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[Display omitted] The quest for efficient hydrogen production highlights the need for cost-effective and high-performance catalysts to enhance the electrochemical water-splitting process. A significant challenge in developing self-supporting catalysts lies in the high cost and complex modification of traditional substrates. In this study, we developed catalysts featuring superaerophobic microstructures engineered on microspherical nickel-coated Chinese rice paper (Ni-RP), chosen for its affordability and exceptional ductility. These catalysts, due to their microspherical morphology and textured surface, exhibited significant superaerophobic properties, substantially reducing bubble adhesion. The nickel oxy-hydroxide (NiO x H y) and phosphorus-doped nickel (PNi) catalysts on Ni-RP demonstrated effective roles in oxygen evolution reaction (OER) and hydrogen evolution reaction (HER), achieving overpotentials of 250 mV at 20 mA cm−2 and 87 mV at −10 mA cm−2 in 1 M KOH, respectively. Moreover, a custom water-splitting cell using PNi/Ni-RP and NiO x H y /Ni-RP electrodes reached an impressive average voltage of 1.55 V at 10 mA cm−2, with stable performance over 100 h in 1 M KOH. Our findings present a cost-effective, sustainable, and easily modifiable substrate that utilizes superaerophobic structures to create efficient and durable catalysts for water splitting. This work serves as a compelling example of designing high-performance self-supporting catalysts for electrocatalytic applications. [ABSTRACT FROM AUTHOR]

Pursuing oxygen evolution reaction (OER) catalysts with high activity and stability is attracting many researchers. Here, we first designed and synthesized a biphasic three-dimensional structured catalyst of nickel–cobalt sulfide NiCo2S4-NiS2/CFP, which is a nickel–cobalt sulfide composite decorated on carbon fiber paper (CFP) by a one-step hydrothermal method. It exhibited an overpotential of about 165 mV at a current density of 10 mA cm−2 and a small Tafel slope of 81.54 mV dec−1. Furthermore, the long-term stability of the NiCo2S4-NiS2/CFP nanocomposite was 90.0% of the initial current density even after 12 h. The excellent catalytic performance of the NiCo2S4-NiS2/CFP nanocomposite can be attributed to several aspects. Firstly, the petal-like morphology of the NiCo2S4-NiS2 nanocomposite exposes more active sites. Secondly, the stability of the composite catalyst is significantly enhanced by its firm anchoring on the CFP. Thirdly, the catalytic performance was significantly improved by the addition of mixed valence of Ni or Co on the {111} plane of spinel NiCo2S4. Finally, the three-dimensional CFP substrate provides an efficient pathway and a stable integrated structure for the transmission of electrons and ions. Our one-step hydrothermal synthesis method provides a simple and economical way to obtain high-performance and robust OER catalysts. [ABSTRACT FROM AUTHOR]

Efficient and durable catalysts for the oxygen evolution reaction (OER) are of great importance for energy storage and conversion devices. However, an objective evaluation and fair comparison of different catalysts remain challenging due to the different catalyst loadings and substrates for OER measurements. In this work, we investigated NiFe layer double hydroxide and commercial Ni/NiO catalysts with different loadings and substrates of glassy carbon (GC), porous nickel foam (NF), and carbon paper (CP). The activity, cycling stability, and potentiostatic stability of the catalysts are compared with respect to the loading and substrate. Catalyst loading exhibits a volcano trend with OER activity, while it has little impact on stability. The 3D substrates NF and CP significantly improved the OER activity of the catalysts compared to GC, especially at higher loadings. The consistent degradation trend of the catalysts confirms the validity of using NF or CP as substrates for the stability test. [ABSTRACT FROM AUTHOR]

Developing high-efficiency electrocatalysts for the hydrogen evolution reaction (HER) is of great importance. In this paper, dendrite-free Ni–Cu catalysts were synthesised via one-step pulse electrodeposition under a weak magnetic field (0.5 T). Regardless of the direction of the magnetic field, the ions were affected by the magnetohydrodynamic (MHD) effect, which greatly promoted the mass transfer and dispersion uniformity, and suppressed the uncontrollable agglomeration by electrodeposition. It was found that the nucleation mechanism changed from progressive nucleation under a 0 T magnetic field to instantaneous nucleation under a 0.5 T magnetic field. Large-scale (325 nm, 0 T) dendrite growth on the single-sided plane was successfully suppressed, and replaced by smaller (90 nm, 0.5 T) and uniformly distributed cluster growth around the carbon paper. In addition, the (111) plane was strengthened by the magnetic field. Electrochemical analysis showed that the Ni–Cu catalysts exposed more surface area and exhibited greatly enhanced catalytic activity, which only needed −57.3 mV to deliver the current density of 10 mA cm−2 with a small Tafel slope of 99.4 mV dec−1 in 1 M KOH. Overall, magneto-electrodeposition, especially under weak magnetic field conditions, provides great promise for the preparation of HER catalysts. [ABSTRACT FROM AUTHOR]

It is a great challenge to synthesize efficient electrocatalysts for overall water splitting, especially non‐noble metal catalysts. Herein, one‐dimensional polycrystalline nanoneedles composed of CoO−Co9S8 nano heterostructures, in situ grown on carbon fiber paper are prepared for efficient overall water electrolysis. Due to strong electronic coupling, charge densities of Co2+/Co3+ in Co9S8 and Co2+ in CoO are favorably modified at the interface of CoO and Co9S8, resulting in optimized reaction intermediates absorption and greatly enhanced bifunctional HER/OER activities. CoO−Co9S8/CFP delivers a current density of 10 mA cm−2 in alkaline electrolyte at overpotentials of 184 mV and 270 mV for HER and OER, respectively. When used as electrocatalyst for overall water splitting, it needs a low cell potential of 1.66 V to realize water electrolysis at 10 mA cm−2. This work provides a new strategy to tune the electronic structures of transitional metal active sites via constructing nano heterostructures for efficient water electrolysis. [ABSTRACT FROM AUTHOR]

Transition metal phosphates with hollow structure have attracted substantial attentions as high-performance electrocatalyst for oxygen evolution reaction (OER). However, these electrocatalytic materials need conductive carrier to realize efficient charge transfer and further improve the OER activity. In this work, ZIF-67 derived hollow NiCo phosphate nanocages supported by waste paper-based carbon aerogel (NCP@WPCA) was prepared as high-efficiency and stable electrocatalyst. Benefited from the enhanced electrochemical active surface area and fast gas emission, the NCP@WPCA catalyst exhibits superior OER activity with low overpotential of 351 mV at current density of 10 mA cm−2, along with good stability in alkaline solution. Additionally, the waste paper-based carbon aerogel as the carrier for electrocatalysts achieves low-cost waste reuse. [Display omitted] [ABSTRACT FROM AUTHOR]

High entropy materials (HEM) have been attracting much attention as emerging catalysts for electrochemical water splitting. HEM catalysts have unique properties such as an interesting cocktail effect, broad design space, customizable electronic structure, and excellent entropy stabilization effect compared with single-digit catalysts. This paper provides a comprehensive overview of the use of HEM as a catalyst for hydrogen evolution reaction (HER), oxygen evolution reaction (OER), and water splitting. HEM design strategies including phase structure modulation, defect engineering, electrode configuration engineering, and computational aids are discussed to develop HEM catalysts with high performance and stability. In particular, the importance of density functional theory, high-throughput screening techniques, and machine learning for the discovery and design of HEM catalysts is emphasized. Finally, the challenges and imminent difficulties are prospected, and the corresponding strategies to deal with these challenges are put forward to promote the development of HEM catalysts in the field of electrochemical water splitting. [ABSTRACT FROM AUTHOR]

The development of efficient non-noble metal electrocatalysts for the oxygen evolution reaction (OER) under acidic conditions remains a critical challenge. Herein, we report a N-doped carbonaceous component-engineered Co3O4 (NCEC) catalyst synthesized via the sol-gel method. Dopamine hydrochloride (DA)-derived nitrogen-doped carbonaceous components were found to boost the OER performance of Co3O4. The optimized catalyst can reach an overpotential as low as 330 mV in 1 M H2SO4 at a current density of 10 mA cm-2 and maintains a good long-term stability of 60 hours. In particular, we found that the thermodynamic overpotential was inversely proportional to the content of oxidized N and pyridinic N, whereas it was directly proportional to the pyrrolic-N content. Our experiments and density functional theory (DFT) calculations confirm that the optimized catalyst exhibits enhanced charge transfer and the oxidized N species on Co3O4 is responsible for the high catalytic activity. Our study suggests that the performance of NCEC in acidic media can be further optimized by enhancing the content of oxidized N species. [ABSTRACT FROM AUTHOR]

Hydrogen, as a clean, safe, and efficient energy carrier, is one of the hot energy sources that have attracted much attention. Mo2C, due to the introduction of C atoms, makes the atomic spacing of the Mo lattice decrease and changes the width of the d-band, which makes the electronic properties of Mo2C similar to that of Pt noble metals, exhibiting excellent electrochemical hydrogen precipitation performance. MoS2, due to its special crystal structure and tunable electronic structure, has been widely studied. In this paper, Mo2C nanoparticles were prepared by high-temperature carbonization, and then two-dimensional layered MoS2 were be loaded on Mo2C nanoparticles by the hydrothermal method to synthesize Mo2C/MoS2 composite catalysts. Their electrochemical hydrogen precipitation (HER) performance under acidic conditions was tested. The above catalysts were also characterized by modern material testing methods such as XRD, SEM, TEM, and XPS. The results showed that the composite catalysts exhibited the most excellent electrochemical hydrogen precipitation performance at Mo2C/MoS2-3, with the lowest overpotential at a current density of 10 mA cm−2, Tafel slope, and electrochemical impedance. At the same time, the electrochemically active area was dramatically enhanced, with good stability under prolonged testing. The catalytic activity was significantly improved compared with that of Mo2C and MoS2. The characterization and experimental results indicate that the heterogeneous structure of Mo2C and MoS2 formed a built-in electric field between the two, which accelerated the electron transfer efficiency and provided more active sites. The Mo2C/MoS2 composite catalyst is a low-cost, easy-to-prepare, and high-efficiency electrochemical hydrogen precipitation catalyst, providing a new idea for developing green and clean energy. [ABSTRACT FROM AUTHOR]

It is highly attractive to develop a photoelectrochemical (PEC) sensing platform based on a non-noble-metal nano array architecture. In this paper, a PEC hydrogen peroxide (H2O2) biosensor based on Ni/WS2/WC heterostructures was synthesized by a facile hydrothermal synthesis method and melamine carbonization process. The morphology, structural and composition and light absorption properties of the Ni/WS2/WC catalyst were investigated by scanning electron microscopy (SEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and UV–visible spectrophotometer. The average size of the Ni/WS2/WC nanosheets was about 200 nm. Additionally, the electrochemical properties toward H2O2 were studied using an electrochemical workstation. Benefiting from the Ni and C atoms, the optimized Ni/WS2/WC catalyst showed superior H2O2 sensing performance and a large photocurrent response. It was found that the detection sensitivity of the Ni/WS2/WC catalyst was 25.7 μA/cm2/mM, and the detection limit was 0.3 mmol/L in the linear range of 1−10 mM. Simultaneously, the synthesized Ni/WS2/WC electrode displayed excellent electrocatalytic properties in hydrogen evolution reaction (HER), with a relatively small overpotential of 126 mV at 10 mA/cm2 in 0.5 M H2SO4. This novel Ni/WS2/WC electrode may provide new insights into preparing other efficient hybrid photoelectrodes for PEC applications. [ABSTRACT FROM AUTHOR]

Synthesiszing highly catalytically active and stable non noble metal oxygen evolution reaction (OER) catalysts with controlled coordination environments at room temperature and probing the relationship between coordination environments and active centers remain challenging. Herein, a series of monomeric particles composed of different coordination environments, Fe–(NH2)4–C, Fe–(NH2)3/OH–C, Fe–(NH2)/(OH)3–C and Fe–(NH2)2/(OH)2–C, were synthesized by means of the response of chitosan salt (HACC) ionomers to pH values in solution at room temperature. The experimental results show that the active center of amine catalysts enables them to exhibit enhanced performance with a low overpotential of 255 mV at 10 mA cm−2 maintaining favorable stability (only 1.3% loss of current density after 12 h) for the OER in a low amino coordination environment (Fe–NH2/(OH)3–C). Therefore, the selection of a suitable coordination environment is the key to the synthesis of efficient and highly stable ionomer-based catalysts. This work provides a practical reference for the design of efficient catalysts in the future. [ABSTRACT FROM AUTHOR]

During the past few years, single‐atom catalysts (SACs) have attracted considerable attention in electrolysis due to their outstanding catalytic performance and efficient atomic utilization. SACs exhibit a simple structure, high catalytic activity, consistent scaling relationships for single sites, and low metal content but their practical applications are still limited. Dual single‐atom catalysts (DACs), which feature excellent selectivity, high atomic utilization efficiency, and remarkable stability, are emerging as new frontiers in heterogeneous electrocatalysis. They increase catalytic activity by promoting synergistic effects between metal‐active sites. In this paper, we present a comprehensive overview of the latest developments in dual‐atom catalysts for oxygen evolution reaction (OER) and oxygen reduction reaction (ORR). In addition, we explore the differences between homonuclear and heteronuclear configurations, the emergence of single/dual‐site metal catalysts, and the methods currently used for their synthesis. Lastly, this review discusses several perspectives for advancing the development of dual‐atom catalysts for OER and ORR electrocatalysis. [ABSTRACT FROM AUTHOR]

NiO-based materials hold great promise as oxygen evolution reaction (OER) catalysts owing to their high intrinsic OER activity and good chemical stability. Herein, Ni/NiO/C hollow microspheres with high activity were successfully fabricated through a facile one-step mist chemical vapor deposition (mist-CVD) process using ethanolamine and nickel chloride as precursors. The high-temperature pyrolysis of the organic precursor yields a significant quantity of gas, leading to a rapid increase in pressure within the droplet, which prompts the nanoparticles to aggregate on the surface of the droplet and form a hollow structure. The crystal phase and morphology of the samples can be modulated through optimizing the decomposition temperature, and particularly, Ni/NiO/C porous hollow microspheres synthesized at 600 °C (Ni-600) presented the best OER activity, exhibiting an overpotential at 10 mA cm−2 (η10) of 286.4 mV and a Tafel slope of 54.8 mV dec−1. The outstanding OER electrocatalytic performance of Ni/NiO/C hollow microspheres is ascribed to the improved electronic conductivity facilitated by the existence of metallic Ni and amorphous C, coupled with the relatively large specific surface area derived from the unique hollow structure. [ABSTRACT FROM AUTHOR]

As a dual-functional catalyst for the hydrogen evolution reaction (HER) and the oxygen evolution reaction (OER), Ru clusters have great potential, but there are certain difficulties regarding their stability on the substrate and the tunability of their electronic environment. Here, the S doped graphited biochar aerogel electrocatalyst was designed and synthesized using terrestrial lignin and algal polysaccharide as a carbon substrate. The Ru clusters were anchored on the S-doped carbon aerogel (P-Ru/SC) by carefully designing the Ru-S bond via a novel plasma assisted high temperature carbonization treatment. The optimized P-Ru/SC-2 catalyst exhibits excellent electrocatalytic performance for the HER and OER, achieving ultra-small overpotentials of 119.6 mV and 193.4 mV at 10 mA cm-2. The dual-electrode requires only 1.47 V to reach 10 mA cm-2. It is worth noting that a large number of S sites on graphited carbon can strongly interact with the Ru clusters, significantly improving the catalytic activity and stability for the HER and OER. [ABSTRACT FROM AUTHOR]

Interfacial engineering emerges as a potent strategy for regulating the catalytic reactivity of metal phosphides. Developing a facile and cost-effective method to construct bifunctional metal phosphides for highly efficient electrochemical overall water splitting remains an essential and challenging issue. Here, a multiphase transition metal phosphide is constructed through the direct phosphorization of a Ni–Co metal–organic framework grown on nickel foam (Ni–Co-MOF/NF), which is prepared by utilizing nickel foam as conductive substrate and nickel source. The resulting transition metal phosphide manifests a pillar-layered morphology, wherein CoP, Ni2P, and Ni5P4 nanoparticles are embedded within each carbon sheet and these carbon sheets assemble into a pillar-shaped structure on the nickel foam (Ni2P–Ni5P4–CoP–C/NF). The heterogeneous Ni2P-Ni5P4–CoP–C/NF with multiple interfaces serves as a highly efficient bifunctional electrocatalyst with overpotentials of −100 mV and 293 mV in the hydrogen evolution reaction and oxygen evolution reaction, respectively, at 50 mA cm−2 in alkaline media. This superior catalytic performance should mainly be ascribed to its enriched active centers and multiphase synergy. When directly applied for alkaline overall water splitting, the Ni2P–Ni5P4–CoP–C/NF couple demonstrates satisfactory activity (1.55 V @10 mA cm−2) along with sustained durability over 18 hours. This method brings fresh enlightenment to the economical and controllable preparation of multi-metal phosphides for energy conversion. [ABSTRACT FROM AUTHOR]

Controllable and scalable preparation of electrocatalyst materials holds significant importance for their practical application. Magnetron sputtering is a highly effective synthesis method, known for its producing uniform films and allowing easy control of component compositions. In this paper, we propose an in-situ synthesis method for layered double hydroxide (LDH) electrocatalysts through sacrificing magnetron sputtered films. The resulting FeCo-LDH catalyst demonstrated a low overpotential of only 300 mV at 10 mA·cm−2. Furthermore, we conducted spectroscopic analysis to investigate the surface changes of the catalysts during the oxygen evolution reaction (OER) process. Our findings indicated that the formation of Co oxyhydroxides plays a beneficial role in enhancing the catalytical performance of the FeCo-LDH for OER reaction. This restructuring strategy of converting a magnetron-sputtered sacrificial film into a catalytical LDH introduces a new avenue to the synthesis of transition metal-based electrocatalysts. [ABSTRACT FROM AUTHOR]

In this paper, a waxberry‐like MnS/Ni3S4 composite catalyst was designed and synthesized. In this coating structure, MnS is located inside and Ni3S4 is wrapped on the surface to form a spherical structure. This structure makes the material show excellent stability in the electrocatalytic process. The diffusion staggered region structure formed at the two‐phase interface greatly enhances the synergistic interaction between MnS and Ni3S4. At the same time, the defects and vacancies formed by the diffusion mechanism at the interface of the two phases increase the active site and improve the interfacial electron transfer kinetics. Therefore, MnS/Ni3S4 composites showed good catalytic performance for ORR/OER. At 10 mA cm−2, the overpotential of it is only 320 mV, and the half‐wave potential can reach 0.81 V. The catalyst also exhibited extraordinary cycle stability and small voltage gap when used as cathode of Zn‐air batteries. When the current density is 3 mA cm−2, the cyclic discharge can be stable for 400 h and the voltage difference between the front and back does not increase more than. When the current density increases to 5 mA cm−2, the cyclic charge and discharge can be stable for more than 300 h. [ABSTRACT FROM AUTHOR]

Au@NiO nanotube arrays were prepared on carbon paper through orderly electrodeposition of ZnO nanorods, Au and NiO, followed by removing ZnO. The morphology and composition of the nanotubes were characterized using scanning electron microscopy, transmission electron microscopy, x-ray diffractometry and x-ray photoelectron spectroscopy. Cyclic voltammetry and amperometric detection were applied to analyze the electrochemical performance of the obtained materials. The Au@NiO nanotubes displayed highly improved electrocatalytic activity for glucose oxidation than that of NiO nanotubes. The optimized Au@NiO nanotube arrays demonstrated excellent glucose sensing performance with a high sensitivity of 5536.2 μA mM−1 cm−2, a wide linear range of 1–6000 μM and a lower detection limit of 0.25 μM. In addition, the Au@NiO nanotube sensors also revealed the good feasibility of glucose detection for real serum samples. The enhanced glucose sensing performance of Au@NiO nanotubes may be due to the bifunctional effect of Au (increasing the charge transfer and acting as direct electrocatalyst for glucose oxidation). The electrodeposition of the Au@NiO nanotube arrays may provide a promising strategy for preparing non-enzymatic glucose sensing materials. [ABSTRACT FROM AUTHOR]

The design of low-cost and high-performance bifunctional catalysts for the hydrogen evolution reaction (HER) and the oxygen evolution reaction (OER) is of great significance for overall water splitting. Herein, RuNi single atom alloy (SAA) decorated on reduced graphene oxide (RuNi@rGO) was synthesized by a facile strategy for use as a bifunctional HER/OER catalyst. The as-obtained RuNi@rGO catalyst exhibits outstanding electrocatalytic activities with an ultralow overpotential for the HER (15 mV) and the OER (240 mV) at a current density of 10 mA cm−2. Density functional theory (DFT) calculations demonstrate that the introduction of Ru single atoms can evidently change the electron distribution and coordination environment around Ni, and reduce the intermediate's adsorption free energy of RuNi@rGO, thus facilitating the HER/OER catalytic rate. Moreover, when used as the cathode and anode of a two-electrode system, the RuNi@rGO-based water splitting device exhibits a low potential of 1.52 V at a current density of 10 mA cm−2, as well as a high faradaic efficiency almost up to 100%, making RuNi@rGO bifunctional electrocatalysts attractive for energy storage and conversion. [ABSTRACT FROM AUTHOR]

The wide application of lithium-ion batteries (LIBs) for electric vehicles forebodes a future decommissioning tide of spent LIBs. Therefore, the recycling of spent LIBs has garnered significant attention, primarily due to the scarcity of resources and the detrimental effects of environmental pollution. However, traditional recycling technologies such as pyrometallurgy and hydrometallurgy methods are limited by their high energy consumption, high pollution, and complicated separation processes. Herein, we propose a novel and general approach to convert a series of spent LiNi1−x−yCoxMnyO2 (NCM) cathodes into Ni–Co–Mn hydroxide (NCM-OH) catalysts for the oxygen evolution reaction (OER) using deep eutectic solvents to extract valuable metals, followed by an in situ precipitation process using oxalic acid and a final self-templating process in an alkaline solution. The NCM-OH catalyst obtained from the spent LiNi0.33Co0.33Mn0.33O2 cathode is found to possess a nanoflake-assembled microrod structure with a large surface area (385.8 m2 g−1) and high porosity, which is endowed with abundant active sites and gas channels for the electrocatalytic reaction and mass transfer process. As a result, the NCM-OH catalyst for the oxygen evolution reaction exhibits a low overpotential of 273 mV at a current density of 10 mA cm−2 with a Tafel slope of 50.46 mV dec−1 as well as satisfactory stability. The effect of the composition on the catalytic performance is also evaluated by comparing different Ni1−x−yCoxMny hydroxide catalysts derived from commercially prevailing spent cathodes. This work provides a promising strategy for recycling spent LIBs into electrocatalyst materials for the OER. [ABSTRACT FROM AUTHOR]

Proton exchange membrane water electrolysis (PEMWE) can be coupled with renewable energy power generation technology and is considered to be a highly promising hydrogen production technology. However, the acidic electrolyte environment, as well as the numerous sulfonic acid groups on the proton exchange membrane surface, can seriously corrode the oxygen evolution reaction (OER) catalyst and even cause deactivation. To develop an efficient acidic OER catalyst, the IrOx/WO3 heterostructure OER catalyst was prepared by a hydrothermal-calcination method. The coordination environment of IrOx was regulated through the electronic rearrangement effect, improving the OER activity and stability of the catalyst in acidic media. The prepared IrOx/WO3 exhibits excellent OER activity in 0.5 M H2SO4, with an overpotential of only 260 mV to achieve a current density of 10 mA cm−2 and a mass activity of 176.8 A gIr−1. It can stably operate for over 12 hours at a current density of j = 10 mA cm−2. [ABSTRACT FROM AUTHOR]

[Display omitted] • Bifunctional catalyst Fe[ Pc (I) 4 ] + Ni[ Pc (I) 4 ]@NC PDI for ORR and OER is synthesized. • The NC PDI with 2D structure and superior stability was used as support. • Iodine groups in TM[ Pc (I) 4 ] creates a built-in electric field to enhance catalysis. • The synergistic effect of Fe[ Pc (I) 4 ]/Ni[ Pc (I) 4 ] enhances the catalytic performance. • The catalyst has superior performance for ORR/OER in rechargeable Zn-air batteries. In this paper, we report on the preparation and catalysis of a bifunctional molecular catalyst (Fe[ Pc (I) 4 ]+Ni[ Pc (I) 4 ]@NC PDI) for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) in rechargeable Zn-air batteries. This catalyst is prepared by self-assembling tetraiodo metal phthalocyanines (Fe[ Pc (I) 4 ] and Ni[ Pc (I) 4 ]) on a 2D N -doped carbon material (NC PDI) through π-π interactions. The introduction of iodine groups in the edge of phthalocyanines controls the density of electron cloud and electrostatic potential around Fe-N/Ni-N sites and constructs a built-in electric field that facilitates directional transport of charges, enhancing the catalytic activity of the catalyst. Density functional theory (DFT) calculations support this mechanism by showing a reduced energy barrier for the ORR rate-determining step (RDS). The Fe[ Pc (I) 4 ]+Ni[ Pc (I) 4 ]@NC PDI exhibits excellent performance outperforming 20 wt% Pt/C and single-molecule self-assembled Fe[ Pc (I) 4 ]@NC PDI and Ni[ Pc (I) 4 ]@NC PDI , with a half-wave potential of E 1/2 = 0.940 V in the ORR process under alkaline condition. During the OER process, Fe[ Pc (I) 4 ]+Ni[ Pc (I) 4 ]@NC PDI exhibited a low overpotential of 298 mV at 10 mA cm−2 under the alkaline condition, which is much better than RuO 2 , Fe[ Pc (I) 4 ]@NC PDI and Ni[ Pc (I) 4 ]@NC PDI. The catalyst also demonstrates excellent catalysis and durability in rechargeable Zn-air batteries. This work provides a simple and specific method to develop efficient multifunctional molecular electrocatalysts. [ABSTRACT FROM AUTHOR]

The synthesis of highly efficient NiFe-layered double hydroxides (NiFe-LDHs) to catalyze the oxygen evolution reaction (OER) is urgent and challenging. Herein, NiFe–FeCl3-x and NiFe–FeCl2-x samples (where FeCl3 and FeCl2 represent the Fe sources and x represents the imposed reaction time: 6, 12, and 24 h) were prepared via one-pot hydrothermal synthesis using Fe sources characterized by Fe(III) or Fe(II) valence states. In the presence of triethanolamine, when FeCl3 was used as the Fe source, pure NiFe-LDH was obtained, whose crystallinity increased with increasing hydrothermal treatment time. In contrast, when FeCl2 was used as the Fe source, a mixture of NiFe-LDH, Fe2O3, and trace amounts of Fe3O4 was obtained. The content of NiFe-LDH in the mixture increased under longer hydrothermal treatment and NiFe–FeCl3-x catalysts exhibited better OER performance than NiFe–FeCl2-x catalysts. Specifically, NiFe–FeCl3-6 afforded the highest OER performance with an overpotential of 246.8 mV at 10 mA cm−2 and a Tafel slope of 46.1 mV dec−1. Herein, we investigated the effects of the valence state of Fe precursors on the structures and OER activities of the prepared catalysts; the mechanism of NiFe-LDH formation via hydrothermal synthesis in the presence of triethanolamine was also proposed. [ABSTRACT FROM AUTHOR]

Non-noble metal-based bifunctional electrocatalysts may be a promising new resource for electrocatalytic water-splitting devices. In this work, transition metal (cobalt)-incorporated graphitic carbon nitride was synthesized and fabricated in electrodes for use as bifunctional catalysts. The optimum catalytic activity of this bifunctional material for the hydrogen evolution reaction (HER), which benefitted at a cobalt content of 10.6 wt%, was promoted by the highest surface area and conductivity. The activity achieved a minimum overpotential of ~85 mV at 10 mA/cm2 and a Tafel slope of 44.2 mV/dec in an acidic electrolyte. These values of the HER were close to those of a benchmark catalyst (platinum on carbon paper electrode). Moreover, the kinetics evaluation at the optimum catalyst ensured the catalyst flows (Volmer–Heyrovsky mechanism), indicating that the adsorption step is rate-determining for the HER. The activity for the oxygen evolution reaction (OER) indicated an overpotential of ~530 mV at 10 mAcm−2 and a Tafel slope of 193.3 mV/dec, which were slightly less or nearly the same as those of the benchmark catalyst. Stability tests using long-term potential cycles confirmed the high durability of the catalyst for both HER and OER. Moreover, the optimal bifunctional catalyst achieved a current density of 10 mAcm−2 at a cell voltage of 1.84 V, which was slightly less than that of the benchmark catalyst (1.98 V). Thus, this research reveals that the present bifunctional, non-noble metallic electrocatalyst is adequate for use as a water-splitting technology in acidic media. [ABSTRACT FROM AUTHOR]

It is highly desirable for porous coordination polymers (PCPs), including metal–organic frameworks (MOFs) and Prussian blue analogues (PBAs), to retain their intrinsic characteristics in electrocatalysis, instead of being used as precursors or templates for further total conversion to other compounds via high-temperature calcination. Here, a S-treated two-dimensional (2D) CoFe bimetallic PBA grown on carbon fiber paper (CFP) (named S-CoFe-PBA/CFP) is assembled and applied as a highly efficient oxygen evolution reaction (OER) electrocatalyst in 1 M KOH. The resultant S-CoFe-PBA/CFP demonstrates significantly improved OER catalytic activity; overpotentials of only 235, 259, and 272 mV are needed to drive current densities of 10, 50, and 100 mA cm−2, respectively, with a super low Tafel slope of 35.2 mV dec−1. Even more noteworthy, a current density of 90 mA cm−2 can be achieved when a potential of 1.5 V vs. RHE is applied, which is 6.4 times higher than that of commercial Ir/C in the same environment. The outstanding electrocatalytic performance can be ascribed to two reasons caused by the S-treatment process. On one hand, H+ from intermediates of *OH and *OOH can be captured by –SOx distributed on the surface of the catalyst, thus accelerating the breaking of O–H; on the other hand, partial phase transformation of CoFe-PBA leads to the in situ formation of amorphous CoSx nanogauze on the surface, and the resultant electronic interactions between the two phases contribute much to the improvement of charge transfer and adsorption for OER intermediates. This work provides a new avenue for the design of highly efficient PCP-based OER electrocatalysts. [ABSTRACT FROM AUTHOR]

The rational design of high-efficiency electrocatalysts for application in water oxidation in alkaline media remains a great challenge. In this paper, Ni3+-rich nanograss-like Mo-doped Ni3S2/NiS/VS arrays grown on nickel foam (denoted as Mo-NiVS@NF) have been successfully constructed through a hydro/solvothermal method. Interestingly, Mo-NiVS@NF exhibits superior catalytic OER performance, needing an overpotential of 217 mV to drive a current density of 10 mA cm−2, outperforming most previously reported NiS-based electrocatalysts. The result indicates that the Ni3+-rich active sites caused by the modulation of the electronic structure environment via the introduction of V and high-valency Mo play an important role in the high activity for the OER. Moreover, this catalyst shows high long-term electrochemical durability. [ABSTRACT FROM AUTHOR]

The potential of converting traditional biomass into low-cost HER catalysts has broad application prospects. In this paper, fungus is used as a carbon-based carrier. The bimetallic catalyst RuM-C (M = V, Mo, W, Zn, Cu) was synthesized under inert gas protection at high temperature. The order of electrocatalytic activity is RuV-C > RuZn-C > RuW-C > RuMo-C > Ru-C > RuCu-C > BF-C, which indicates that RuV-C exhibits excellent HER activity. Due to its irregular sheet structure, the specific surface area of the catalyst is increased. Impressively, it exhibits extremely high catalytic activity for HER in 1 M KOH due to favorable kinetics and excellent specific activity. Consequently, the prepared RuV-C exhibited excellent and stable HER activity compared Ru-C with a low overpotential of 65.78 mV at the current densities of 10 mA cmâˆ'2 and Tafel slope of 45.26 mV decâˆ'1. The potential only decreased by 88 mV after 24 h of continuous testing, which indicates that the catalyst has outstanding stability. This work will provide positive inspiration for the promotion of a new Ru-based biomass HER electrocatalyst. [ABSTRACT FROM AUTHOR]

CP@NC-CoFe 2 O 4 /C as catalysts for OER: we covered a polyaniline nanowire array on carbon paper by a electrochemical polymerization method, directly grown MOF-74-Co/Fe on its surface and pyrolyzed to form the CoFe 2 O 4 /C supported on nitrogen-doped carbon nanoarray meterial, which is prepared a highly active and stable OER catalyst. High specific surface area, high utilization of the catalyst, enhanced electron transport characteristics and retention characteristics of the original carbon paper characteristics ensure excellent OER activity. Our results show great promise for developing OER catalysts as precious metal substitutes for PANI and MOFs complexes through a low-cost, scalable method. [Display omitted] • Polyaniline nanowire array was covered on carbon paper, directly grown MOF-74-Co/Fe on its surface. • The presence of PANI nanowire arrays also retains the original properties of carbon paper. • The unique 3D nano-array structure enhance the OER catalytic efficiency. • DFT reveals the main surface adsorbent is OH*, and surface Co atoms are the main active sites. Here, we covered a polyaniline nanowire array (denoted as PANI) on carbon paper (denoted as CP) by a electrochemical polymerization method, directly grown MOF-74-Co/Fe on its surface and pyrolyzed to form the CoFe 2 O 4 /C supported on nitrogen-doped carbon nanoarray materials (denoted as NC-CoFe 2 O 4 /C@CP), which is prepared a highly active and stable OER catalyst. PANI can not only be used as a "binder", grow MOF on its surface and cover the carbon paper, but also improve the conductivity and stability of the material by forming nitrogen-doped carbon after pyrolysis. And its unique 3D nano-array structure not only greatly increases the surface area, but also provides more attachment sites for CoFe 2 O 4 , thereby accelerating electron transport and improving OER performance. High specific surface area, high utilization of the catalyst, enhanced electron transport characteristics and retention characteristics of the original carbon paper characteristics ensure excellent OER activity. The final sample exhibits outstanding activity for OER in alkaline solution, accompanied by a low onset potential about 1.52 V (vs reversible hydrogen electrode), and the small Tafel slope of 70 mV dec−1. In particular, after 21600s, the current drop is negligible, which is means that the NC-CoFe 2 O 4 /C@CP catalyst has the high stability. Density Functional Theory (DFT) calculation reveals the main surface adsorbent of CoFe 2 O 4 is OH*, and the surface Co atoms are the main active sites. [ABSTRACT FROM AUTHOR]

• In situ XANES analysis coupled with CV measurements identified the activation and two-stage degradation mechanisms of Ni-LDH catalysts in OER. • First and second stages of degradation are due to isolation of γ-NiOOH and overcharge of β-NiOOH. • Use of high-density carbon substrate for Ni(OH) 2 allowed a high and stable activity under potential changes. The activation and degradation mechanism of Ni-LDH catalysts electrodeposited on low and high-density carbon papers for the oxygen evolution reaction (OER) in alkaline media was investigated using in situ X-ray absorption near-edge structure (XANES) spectroscopy coupled with CV cycles in a potential range of 0–0.9 V (vs Hg/HgO), which allowed proposing two-stage degradation mechanisms with respect to cyclic voltammetry (CV) cycles. The electrodeposited α-Ni(OH) 2 is firstly transformed to γ-NiOOH as an active phase in OER. In the reducible potential region, however, γ-NiOOH was partially reduced to β-Ni(OH) 2 , isolating the rest, which is the first stage of degradation. In the following anodic potential region, β-Ni(OH) 2 is readily converted to β-NiOOH, which is mostly reversible, but only a small portion of β-NiOOH is overcharged to unstable γ-NiOOH, being responsible for the second stage degradation. It was noted that Ni(OH) 2 catalysts electrodeposited on a low-density carbon paper (Ni-LC) underwent a severe degradation in the first stage, losing at least 56.9 % current density at 0.65 V (vs Hg/HgO), followed by a steady degradation in the second stage, while the use of a high-density carbon substrate (Ni−HC) effectively improved redox stability, maintaining a minimal loss of overpotential less than 5%, particularly with the second stage degradation being negligible even under potential changes, providing an important insight into designing durable and active Ni-LDH catalysts for the OER. [ABSTRACT FROM AUTHOR]

We used sodium hydroxide-mediated approach and tannic acid etching to prepare hollow structured trimetallic MOF-derived CoFeNi/Z-P NC nanocomposites. Remarkably, the resulting CoFeNi/Z-P NC nanocomposites have large specific surface area and mesoporous structure, making their active sites more accessible and mass transfer more effective. More complex trimetallic components provide greater possibilities for further improving electrocatalytic performance. The CoFeNi/Z-P NC nanocomposites demonstrate notable enhancements for the OER, and 10 mA cm−2 current density is achieved at a low overpotential of 244 mV, with a low Tafel slope of 66.2 mV dec−1 and have good stability in alkaline solutions. In addition, as a cathode material for overall alkaline water splitting, CoFeNi/Z-P NC is better than RuO2 with longer cycling stability. [ABSTRACT FROM AUTHOR]

The exploitation of highly active and stable catalysts for reduction of CO2 and water oxidation is one of the approaches to facilitate scalable and sustainable CO2 reduction potentially at the industrial scale. Herein, a feasible strategy to rationally build an overall CO2 + H2O electrocatalytic reaction device is the preparation and matchup of a high-performance CO2 reduction catalyst and low-cost and highly active oxygen anode catalyst. A heterostructured nanosheet, γ-NiOOH/NiCO3/Ni(HCOO)2, exhibited superior catalytic activity in the oxygen evolution reaction, and was integrated with CoPc/Fe–N–C to build an overall CO2 + H2O cell with a current density of 10 mA cm−2 at a very low cell voltage of 1.97 V, and the faradaic deficiency of CO2 to CO was maintained at greater than 90% at 1.9 V. [ABSTRACT FROM AUTHOR]

Developing non-precious metal catalysts for the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER) is critical for Zn–air batteries. Herein, using NaCl and ammonium oxalate as templates to prepare a hierarchical porous Fe–N–C catalyst using an inorganic salt melting strategy is proposed. The prepared Fe–N–C-x catalysts have a hierarchical porous structure that increases the specific surface area, improves the exposure of a number of active sites and enhances the chance of contacting active sites. The structure change of a leaf-shaped zeolitic imidazolate framework (ZIF-L) during high-temperature pyrolysis was used to self-catalyze the growth of carbon nanotube structures, forming a structure of carbon nanotubes including Fe nanoparticles to provide additional active sites and reduce the aggregation of metal particles. From the perspective of economy and electrochemical performance, it is found that when the addition amount of NaCl and ammonium oxalate respectively is 2 g, the electrochemical performance of the ORR, OER and Zn–air batteries is better, and the preparation cost of the catalyst is more affordable. This strategy of forming hierarchical porous Fe–N–C catalysts by self-catalytic growth of Fe, N co-doped CNTs using inorganic salts provides a new design idea for the preparation of new hierarchical porous electrocatalysts. [ABSTRACT FROM AUTHOR]

It is widely acknowledged that interface engineering strategies can significantly enhance the activity of catalysts. In this study, we developed a CoMoP nanoarray directly grown in situ on a nickel foam (NF) substrate, with the interface structure formed through the electrodeposition of MnOxHy. The resulting heterostructure MnOxHy/CoMoP/NF exhibited remarkable hydrogen evolution reaction (HER) activity, achieving overpotentials as low as 61 and 138 mV at 10 and 100 mA cm−2, respectively. Moreover, MnOxHy/CoMoP/NF demonstrated efficient oxygen evolution reaction (OER) activity with an overpotential of 330 mV at 100 mA cm−2. Remarkably, MnOxHy/CoMoP/NF maintained its catalytic properties and structural integrity even after working continuously for 20 h facilitating the HER at 10 mA cm−2 and the OER at 100 mA cm−2. The Tafel slopes of the HER and OER were determined to be as small as 14 and 55 mV dec−1, respectively, confirming that the coupled interface conferred fast reaction kinetics on the catalyst. When applied in overall water splitting, MnOxHy/CoMoP/NF delivered a voltage of 1.91 V at 100 mA cm−2 with excellent stability. This study demonstrated the feasibility of utilizing a simple electrodeposition technique to fabricate a heterogeneous structure with bifunctional catalytic activity, establishing a solid foundation for diverse industrial applications. [ABSTRACT FROM AUTHOR]

Summary: Obstacles to the efficient operation of rechargeable aluminum‐air batteries include slow oxygen reduction reaction (ORR), slow kinetics, and large overpotential of oxygen evolution reactions (OER). An effective solution is to develop a new bifunctional electrocatalyst that is effective for both the ORR/OER processes. In this study, we prepared the α‐MnO2/Co3O4 bifunctional composite catalyst by the in situ generation of Co3O4 nanoparticles on α‐MnO2 nanorods. ORR/OER catalytic activity and structures of the prepared catalysts have been investigated systematically. Compared with single‐component α‐MnO2 nanorods and Co3O4 particles catalyst, the α‐MnO2/Co3O4 composite catalyst possesses the smallest average pore diameter (11.84 nm), and the largest specific surface area (41.34 m2 g−1), which is due to the restriction of the growth of Co3O4 particles by α‐MnO2 nanorods. Besides, during the ORR process, the α‐MnO2/Co3O4 composite catalyst shows the most positive onset potential of 0.833 V, the most positive half‐wave potential of 0.760 V, and the biggest limiting current density of 3.881 mA cm−2. Meanwhile, during the OER process, the composite catalyst exhibits the lowest onset potential of 1.630 V, the lowest overpotential of 554 mV, and the biggest limiting current density of 24.590 mA cm−2. Furthermore, the α‐MnO2/Co3O4‐assembled aluminum‐air battery (AAB) delivers the best cycling performance. Our work provides an idea for optimizing the bifunctional catalyst with high ORR/OER activity and low cost used in secondary AAB. Highlights: A novel α‐MnO2/Co3O4 bifunctional composite catalyst was prepared successfully.The α‐MnO2/Co3O4 composite catalyst was applied in a rechargeable Al‐air battery.The α‐MnO2/Co3O4 exhibited better ORR/OER catalytic activity than α‐MnO2 and Co3O4.The Al‐air battery using α‐MnO2/Co3O4 catalyst showed excellent cycling performances. Novelty Statement: This is our original work. Neither the entire paper nor any part of its content has been published or has been accepted elsewhere. It is not being submitted to any other journal. [ABSTRACT FROM AUTHOR]

Summary: Catalysts with cobalt (Co) and graphitic carbon hybrid structure are receiving significant attention in various electrocatalysis applications because of their stability and high activities. In addition, the size and the well dispersed distribution of metal active site are some of the most important factors for electrocatalyst. In this paper, we successfully synthesized ultra‐small and well dispersed Co nanoparticle on nitrogen‐doped carbon structure (Co/NC) adding and evaporating a Zinc (Zn) and found the optimized ratio of Co and Zn. We used a bottom‐up method to synthesize catalysts with Co on carbon substrate structure from zeolitic imidazolate frameworks (ZIF). Zinc (Zn) was also added and evaporated by pyrolysis. By addition and evaporation of Zn, Co nanoparticle became smaller and more evenly dispersed. As a result, the OER performance was significantly improved than the catalyst without Zn. Also, an optimized catalyst with abundant uniformly dispersed Co was successfully synthesized by appropriately controlling the ratio of Co and Zn comprising the ZIFs. As the ratio of Zn increased, the size and the amount of Co nanoparticles were decreased, and Co nanoparticles were more evenly dispersed. Furthermore, carbon substrate has more porous structure due to the evaporation of Zn atoms. When the Co:Zn ratio was 1:3, Co/NC showed the best electrocatalytic performance due to optimized active sites and large surface area. The optimized Co/NC showed an overpotential of 1.56 V (vs RHE) to acquire a current density of 10 mA cm−2, which is higher activity than commercial RuO2. We also analyzed the material characterization occurred as the ratio of Zn in ZIF increased, revealing the factors enhancing the OER activity. Optimized Co/NC (Co:Zn = 1:3) exhibited improved OER activity and long‐term and cycle stability in the OER. [ABSTRACT FROM AUTHOR]

In order to obtain platinum-group-metal-free catalysts for the oxygen evolution reaction (OER) and the hydrogen evolution reaction (HER) in alkaline electrolyzers, nitrogen-doped mesoporous carbons were prepared from pyrolysis of two cobalt metal organic frameworks (MOFs), one linear coordination polymer and one complex. The catalyst derived from cobalt 2,3-pyrazinedicarboxylate polymer (700 °C) had a Tafel slope of 90 mV dec−1 and 130 mV dec−1 for the HER and OER respectively, a current density of 10 mA cm−2 was reached at − 0.23 V and 1.56 V vs RHE for the HER and OER respectively. In order to prove the bifunctional catalytic activity towards the overall water splitting, a two electrode electrolyzer was constructed depositing the catalyst on carbon paper. H2 and O2 evolved volumes followed the Faraday law, showing efficiency very close to 100%. The same materials also showed catalytic activity towards the oxygen reduction reaction (ORR), reaching an electron transfer number close to 4 and low H2O2 yields. The acid leached catalyst derived from Cobalt 2,3-pyrazinedicarboxylate polymer (700 °C) reached a ∆E = Ej = 10(OER) −E½(ORR) = 0.80 V, making it an useful oxygen catalyst for metal-air batteries. [ABSTRACT FROM AUTHOR]

In water splitting, the oxygen evolution reaction (OER) performance of transition metal alloy catalysts needs to be further improved. To solve this problem, the method of an external magnetic field was used to improve the OER catalytic performance of the alloy catalyst. In this paper, FeCo alloys with different composition ratios were prepared by an arc melting method, and OER catalysts with different compositions were obtained by annealing treatment. Under the action of a magnetic field, all three groups of catalysts showed a better catalytic performance than those without a magnetic field. The overpotentials of Fe35Co65, Fe22Co78 and Fe15Co85 at a current density of 20 mA cm−2 were reduced by 12 mV, 6 mV and 2 mV, respectively. It is found that, due to the magnetostrictive properties of FeCo alloys, the catalyst itself will generate strain under the action of a magnetic field, and the existence of strain may be the main reason for the enhanced OER performance of the magnetic field. Therefore, this work provides a new idea for the development of magnetic material catalysts and a magnetic field to improve the performance of catalysts. [ABSTRACT FROM AUTHOR]

Perovskite‐based catalysts have received a lot attention as bifunctional oxygen evolution reaction and oxygen reduction reaction (ORR/OER) catalysts in secondary rechargeable zinc–air batteries due to their tunable structure, stability at high current densities, low cost, lightweight, and nontoxicity. This paper investigates a new perovskite material, Sr2TiMnO6 (STMO), for a rechargeable zinc–air battery (ZAB). The crystalline structure, morphology, and adsorption/desorption behavior of STMO are thoroughly studied and investigated their catalytic processes. The perovskite catalyst shows high catalytic activities, durability, and endurance in the alkaline medium, resulting in the power density of 97 mW·cm−2, and a specific capacity of 705.21 mAh·g−1. The rechargeable STMO ZAB exhibited good cycling stability with the current density of 3.5 mA·cm−2 for 6.66 h and low overpotential. The observed results promise STMO to be a viable candidate as a functional (ORR/OER) electrocatalyst which can be successfully used for commercial fuel‐cells and metal air batteries. [ABSTRACT FROM AUTHOR]

The synthesis of electrocatalyst and the electrode preparation were merged into a one‐step process and proved to be a versatile method to synthesize metal oxide electrocatalysts on the conductive carbon paper (CP). Very simply, the metal precursor deposited on the CP was thermally treated by a torch‐gun for just 6 s, resulting in the formation of RuO2, Co3O4, and mixed oxide nanoparticles. The material could be directly used as working electrode for oxygen evolution reaction (OER). Compared with commercial and other state‐of‐the‐art electrocatalysts, the fabricated electrode showed a superior electrocatalytic activity for OER in 1 m HClO4 and 1 m KOH in terms of not only a low overpotential to reach 10 mA cm−2 but also a high current density at 1.6 VRHE with satisfying a long‐term stability. The novel strategy without requiring time‐consuming and uneconomical steps could be expanded to the preparation of various metal oxides on conductive substrates towards diverse electrocatalytic applications. [ABSTRACT FROM AUTHOR]

The oxygen evolution reaction is a key step in controlling the efficiency and stability of water electrolysis. The development of high-efficiency, energy-saving catalysts that can be used at an industrial scale is currently a major challenge. In this paper, the complex reaction of oxalic acid, ferrous chloride, and cobalt chloride in N,N-dimethylacetamide solution is used to generate an oxalic acid complex, which is then glued with polyvinylpyrrolidone and sintered to generate a bimetallic alloy catalyst. According to electrochemical tests, the obtained FeCo-2K30 has excellent activity and stability in alkaline electrolytes. Specifically, FeCo-2K30 has an overpotential of 313 mV at 10 mA cm−2 and a Tafel slope of 58 mV dec−1. Its catalytic performance is comparable to that of noble metal electrocatalysts. [ABSTRACT FROM AUTHOR]

The intelligent design or development of dual‐functional catalysts using non‐precious metals especially for the oxygen evolution reaction (OER) in sustainable energy systems and degradation of organic pollutants is still a difficult and a significant challenge. Furthermore, the development of these catalysts is of great importance in terms of energy security and solution of the environmental problems. To meet these requirements, herein, we describe the synthesis of a Ni‐ion doped Birnessite@Cryptomelane (Ni2+/B@Cr) hybrid structure as a bifunctional efficient catalyst for the OER in neutral media and degradation of dye pollutants. The Ni2+/B@Cr catalyst exhibited a sharp onset potential at 390 mV (vs. RHE) and achieved a current density of 1 mA cm−2 at a low ƞ of 430 mV with a Tafel slope of ~96 mV dec−1. The results of electrochemical impedance spectroscopy (EIS) studies indicated that Ni intercalation into birnessite layer and heterostructure of the hybrid electrocatalyst Ni2+/B@Cr increased the conductivity by lowering the resistance of charge transfer (Rct = 4.82 Ω) and oxygen evolution processes (ROER = 4.13 Ω). The durability assay identified Ni2+/B@Cr as stable electrocatalyst with 10% loss of activity after long‐term stability tests (10 h, under 500‐mV overpotential). In addition, the Ni2+/B@Cr achieved high (86.67 s−1 g−1) and rapid (173 s) catalytic performance for the reduction of methylene blue (MB). Overall, this paper presents a low‐cost production strategy for the design of highly efficient bifunctional catalysts, offering boosted electrocatalytic and degradation performance for water oxidation and organic dye contamination, respectively. [ABSTRACT FROM AUTHOR]

The development of high‐efficiency catalysts for carbon dioxide reduction reaction (CO2RR) and oxygen evolution reactions (OER) is an important strategy to solve the current energy crisis. In this paper, solid‐phase exfoliation and electrostatic self‐assembly strategies are developed to couple ultrathin NiFe‐layered‐double‐hydroxide nanosheets and carbon nanotubes (CNT@NiFe‐LDH NS) as an OER catalyst. Then, NiFe nanoparticles anchored on the N‐doped CNT (CNT‐N‐NiFe) for electrocatalyst of CO2RR is synthesized via pyrolysis of a mixture of CNT@NiFe‐LDH NS and melamine in a nitrogen atmosphere at 750 °C, utilizing the ultrathin NiFe‐LDH NS as a metal source and CNT as the framework. CNT@NiFe‐LDH NS nanohybrid exhibits a better catalytic activity for OER (with an overpotential of 270 mV at the current density of 20 mA cm–2 and remarkably stable durability) than Bulk NiFe‐LDH in 1 m KOH. Moreover, the CNT‐N‐NiFe catalyst exhibits a Faradaic efficiency of ≈82.6% for the reduction of CO2 to CO at −0.7 V (vs reversible hydrogen electrode) with a current density of CO 10.2 mA cm–2. The method of preparing CO2RR catalysts provides a new idea of the preparation of bimetallic CO2RR electrocatalysts. [ABSTRACT FROM AUTHOR]

NiO has been widely studied as a potential Earth-abundant electrocatalyst for the oxygen evolution reaction (OER). Defect engineering and constructing hollow nanostructures are effective methods to improve electrocatalytic performance, so exploring an efficient route to obtain NiO catalysts simultaneously possessing oxygen vacancies and hollow nanostructures is necessary. In this work, core–shell NiO1−x hollow spheres with oxygen vacancies are prepared through a solvothermal strategy followed by thermal treatment under an H2/Ar atmosphere. And the content of oxygen vacancies can be regulated by varying the calcination time. Importantly, the existence of rich oxygen vacancies in NiO and its unique core–shell hollow structure promote water adsorption and enhance charge transfer and thus the core–shell NiO1−x hollow spheres show appealing electrocatalytic performance, demonstrating efficient OER electrocatalysis with an overpotential (η) of 360 mV (at 10 mA cm−2) and Tafel slope of 103.9 mV dec−1 in an alkaline medium. [ABSTRACT FROM AUTHOR]

Powder electrocatalysts for oxygen evolution reactions usually need adhesives for electrocatalytic performance tests, leading to the increase of resistance, reduction of catalyst loading, and easy stripping of the catalyst under long-time or high current operation. In this study, Ce-doped CoFe layered double hydroxides were uniformly grown on nickel foam by a one-step hydrothermal route. A nanostructured self-supported electrode Ce-CoFe-LDH/NF without adhesive was obtained directly, which has a regular nanoneedle morphology with a length of ∼1.2 μm and tip width of ∼20 nm. Adopting Ce3+ ions with a large radius to partially displace Fe3+ ions with a small radius produced lattice distortion and more defects in the host layer of CoFe-LDH, whereby possessing the great potential to enhance catalytic behaviors. Once used as an electrocatalyst for the oxygen evolution reaction, Ce-CoFe-LDH/NF shows an outstanding electrocatalytic performance, including an optimized overpotential of 225 mV at 10 mA cm−2, a decreased Tafel slope of 34.34 mV dec−1, and a low charge transfer impedance of 2.4 Ω in 1 M KOH electrolyte. Moreover, the overpotential of the working electrode increased by only 0.04 V after 24 hours and was maintained at a current density of 50 mA cm−2. These results demonstrate a low-cost strategy compared to using noble metal OER electrocatalysts. Thus, this study highlights a ready universal approach to fabricate high-performance supported catalysts for energy-related applications. [ABSTRACT FROM AUTHOR]

The development and optimization of electrocatalysts is one of the key points to reduce the energy barrier of electrocatalytic water splitting and improve the kinetics of electrocatalytic reactions. It is necessary to develop low-cost, high-performance electrocatalysts with large-scale application prospects. In order to solve this problem, hybrid structured ZnCo2O4@Co3O4 nanowires are successfully synthesized through hydrothermal synthesis and electrodeposition. As electrocatalysts for water splitting, ZnCo2O4@Co3O4 can reach a current density of 50 mA cm−2 at an overpotential of 278 mV for the OER and 166 mV@−10 mA cm−2 for the HER, which could be higher than that of single ZnCo2O4 and Co3O4. At the same time, ZnCo2O4@Co3O4 samples also exhibit a cell voltage of 1.67 V at a high current density of 50 mA cm−2 and superior durability for 50 h. The fabricated product also showcases a specific capacitance of 1316 F g−1 at 1 A g−1. Additionally, the assembled device attains a maximum energy density of 47.3 W h kg−1 at a power density of 1126 W kg−1. Furthermore, density functional theory (DFT) calculation further confirms that the heterostructure can significantly promote Gibbs free energy for hydrogen adsorption. And the significant increase in the density of total states (DOS) also enhances the catalytic activity for the HER. [ABSTRACT FROM AUTHOR]

Designing an excellent OER catalyst in an alkaline environment is severe yet essential for industrial H2 application under the electrochemical technique. This study has achieved multiple modifications on CoN nanowires, the classic OER catalyst, via a facile room-temperature NaBH4 spontaneous hydrolysis. This facile process simultaneously generates oxygen vacancies and robust BN species. It wraps hydrophilic BOx motifs on the OER response CoN nanowires, producing OER active Co–N–B species, increasing active numbers and guaranteeing structural stability. It suggests that a low NaBH4 concentration (0.1 mol L−1) treatment endows CoNNWAs/CC with excellent OER performance and robust structure, which can drive a current density of 50 mA cm−2 with only 325 mV overpotentials with more than 24 hours' durability. Even, the catalyst can drive 1000 mA cm−2 around 480 mV overpotential. This study allows a novel strategy for designing high-performance OER catalysts. [ABSTRACT FROM AUTHOR]

The proton exchange membrane (PEM) water electrolyzer has been considered a versatile approach for practical H2 production. However, the oxygen evolution reaction (OER) in acid media with complicated proton-coupled electron transfer steps possesses sluggish kinetics and high reaction barriers, severely hindering the development of PEM water electrolyzers. Consequently, high-efficient Ru- and Irbased catalysts have always been essential to accelerate the OER rate and lower the reaction barrier in PEM water electrolyzer. Therefore, it is very necessary to construct low-cost catalysts with excellent electrocatalytic performances to replace these noble metal-based OER electrocatalysts. In this review paper, a detailed discussion towards fundamentally comprehending the reaction mechanisms of OER was conducted. Accordingly, we proposed the principles of designing advanced OER electrocatalysts with enhanced performances and lowered costs. After that, recent developments in designing various acidic OER electrocatalysts were summarized. Meanwhile, the available regulation strategies about noble metals, nonprecious metals, and metal-free nanomaterials were presented, which are promising for tuning the electronic structures, boosting the electrocatalytic performances, and reducing the costs of electrocatalysts. We also provided the existing challenges and perspectives of various OER electrocatalysts, hoping to promote the development of PEM water electrolyzers. [ABSTRACT FROM AUTHOR]

WO3 nanowires (NWs) have emerged as a promising alternative electrocatalyst for the photoelectrochemical (PEC) oxygen evolution reaction (OER), due to their nontoxicity, low cost, good stability, and strong photocatalytic oxidation ability. However, a significant challenge is limited by the poor electrical conductivity and the rapid recombination rate of photogenerated carriers. This paper reports a facile and effective way to synthesize the WO3 NWs with oxygen vacancies (Ov-WO3 NWs), which have high PEC OER activity and good stability. Photoelectric measurements indicate that the Ov-WO3 NW-based device shows a good light-harvesting property under visible light and a prolonged photoresponse time. Electrochemical impedance spectra measurements reveal a reduced value of Rct denoting an improved electrical conductivity, which should be responsible for the superior PEC OER performance. Our work provides a strategy for fabricating efficient water-splitting electrodes to help establish rational design principles for future OER catalysts. [ABSTRACT FROM AUTHOR]

The development of highly active electrocatalysts is of great importance toward the practical applications of many meaningful electrocatalytic reactions. In this paper, the synthesis and electrocatalytic properties of a multifunctional ruthenium nickel boride hybrid electrocatalyst are reported for the first time. Compared to pristine nickel boride (Ni‐B) and Ru electrocatalysts, Ru@Ni‐B with trace Ru loading amount of 0.133 mg cm−2 prepared by a simple wet chemical method, shows remarkably improved activity toward the hydrogen evolution reaction, the oxygen evolution reaction, and the glucose oxidation reaction. The electrolytic cell assembled with Ru@Ni‐B/nickel foam electrode as both cathode and anode can deliver 10 mA cm−2 at only 1.42 V for alkaline overall water splitting and 1.24 V for glucose electrolysis. It is further found that the synergistic coupling of ruthenium with nickel boride plays an important role in the superior performance of the hybrid electrocatalyst. [ABSTRACT FROM AUTHOR]

Two-dimensional Ni(OH)2 is a cheap and promising urea oxidation reaction (UOR) catalyst, but its catalytic performance is seriously hampered by fatal disadvantages including sluggish kinetics, limited exposed active sites in the bulk and unsatisfactory stability. Herein, we report a chlorine-anion modified nickel hydroxide nanosheet (Cl–Ni(OH)2) with much better charge transfer, more active centers and improved working stability using an easy-operation method at room temperature. Impressively, the optimal Cl32–Ni(OH)2 catalyst delivers a current density of 106.93 mA cm−2 at 1.6 V vs. RHE and a Tafel slope of 42.37 mV dec−1, much better than those of pristine Ni(OH)2 (20.38 mA cm−2, 100.40 mV dec−1). Moreover, Cl32–Ni(OH)2 exhibits excellent long-term durability over 15 h under 10 mA cm−2. This work provides an efficient catalyst for the UOR and affords a simple method to improve the electrocatalytic activity of two-dimensional catalysts for energy conversion. [ABSTRACT FROM AUTHOR]