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Direct synthesis of large‐area graphene on functional substrates via chemical vapor deposition has become a frontier research stream targeting practical applications. However, the batch production of transfer‐free graphene film with favorable quality and homogeneity remains a grand challenge. Herein, the direct growth of 12‐inch‐sized graphene is demonstrated over fused quartz in a batch manner. The key design of the synthetic route is the construction of a nano‐scale compartment to allow the formation of free molecular flow during growth, as well as to trap the hydroxyl species in situ released from the quartz substrates. Density functional theory calculations reveal that the hydroxyl species help decrease the energy barrier for feedstock decomposition and facilitate the carbon attachment to boost graphene growth. Thus‐prepared graphene possesses excellent optical transmittance (96% ± 1%) and electrical properties (1.22 ± 0.08 kΩ sq‒1). These findings unlock new opportunities for achieving batch production of graphene‐skinned functional materials with practical scalability and quality toward emerging uses. [ABSTRACT FROM AUTHOR]

Direct synthesis of large‐area graphene on functional substrates via chemical vapor deposition has become a frontier research stream targeting practical applications. However, the batch production of transfer‐free graphene film with favorable quality and homogeneity remains a grand challenge. Herein, the direct growth of 12‐inch‐sized graphene is demonstrated over fused quartz in a batch manner. The key design of the synthetic route is the construction of a nano‐scale compartment to allow the formation of free molecular flow during growth, as well as to trap the hydroxyl species in situ released from the quartz substrates. Density functional theory calculations reveal that the hydroxyl species help decrease the energy barrier for feedstock decomposition and facilitate the carbon attachment to boost graphene growth. Thus‐prepared graphene possesses excellent optical transmittance (96% ± 1%) and electrical properties (1.22 ± 0.08 kΩ sq‒1). These findings unlock new opportunities for achieving batch production of graphene‐skinned functional materials with practical scalability and quality toward emerging uses. [ABSTRACT FROM AUTHOR]

The Ni/NiMoO x can be successfully used as both anodic and cathodic electrodes to construct hybrid water splitting system by employing UOR to replace sluggish OER for H 2 generation. [Display omitted] • The Ni/NiMoO x was reconstructed from NiMoO 4 precursor under H 2 /Ar atmosphere. • The Ni/NiMoO x exhibits superior electrocatalytic activities toward UOR, OER, and HER. • The Ni/NiMoO x is employed to assemble a hybrid water splitting cell as both cathode and anode. • DFT results prove that the heterojunction effectively modulates the surface polarization of Ni/NiMoO x , improving its activity for UOR. Electrocatalytic urea oxidation (UOR) has attracted significant interest as a promising anodic half-reaction to replace sluggish oxygen evolution reaction (OER) toward water splitting. However, the activation and decomposition of urea molecule maintains a challenge during electrocatalytic process because of its 6e− oxidation procedure. Herein, Ni nanoparticles decorated NiMoO x nanorod (Ni/NiMoO x) electrocatalyst with abundant heterojunction interfaces is fabricated and the density functional theory (DFT) calculation testifies that the interfaces are favorable for enhancing the conductivity and modulating the surface polarization of Ni/NiMoO x , thus improving its UOR's activity. The Ni/NiMoO x performs superb electrocatalytic capacities toward UOR with a potential of 1.355 V (vs RHE) at 20 mA cm−2, and HER with an overpotential of 98 mV at 10 mA cm−2. A hybrid two-electrode water splitting cell is further assembled via applying the Ni/NiMoO x as both anodic and cathodic electrodes with presence of 0.33 M urea, delivering 50 mA cm−2 at voltage of 1.589 V. The findings help to provide a reliable strategy for rational reconstruction of Ni based metal oxide with rich interfaces for diverse electrocatalytic reactions. [ABSTRACT FROM AUTHOR]

Sluggish sulfur reduction reaction (SRR) kinetics remains a formidable challenge in Li–S electrochemistry. In this sense, the rational design of single‐atom species has become a burgeoning practice to expedite sulfur redox, where the underlying catalytic mechanism otherwise remains elusive. Herein, a class of metal single‐atom modified porous carbon nanofiber films (MSA PCNFs, M = Fe, Co, or Ni), fabricated via a generic synthetic strategy, as mediators to boost SRR kinetics is reported. Throughout electrokinetic measurement and operando instrumental probing, NiSA PCNF is evidenced to harness the catalytic superiority toward the rate‐determining step (i.e., liquid–solid conversion) of the SRR process. Density functional theory (DFT) simulations further reveal that the catalytic features of M–N–C moieties in catalyzing the Li2S precipitation rely heavily upon the coordination environments of adjacent carbon atoms and d‐orbital configurations of metal centers. In response, the thus‐derived S/NiSA PCNF cathode realizes an encouraging areal capacity of 14.12 mAh cm−2 under elevated sulfur loading (10.2 mg cm−2) and lean electrolyte usage (E/S ratio ≈ 5.5 μL mg−1). This work offers insight into the identification of exact catalytic moieties for different transition metal M–N–C single‐atom SRR mediators, showcasing a meaningful guidance and potential impact on Li–S catalysis. [ABSTRACT FROM AUTHOR]

Li metal is regarded as one of the most promising anodes for next‐generation rechargeable batteries. Nonetheless, infinite volume change and severe dendrite growth impede its practicability. To date, unremitting efforts have been devoted to stabilizing Li metal anode via the rational design of 3D current collectors. In this sense, optimizing Li nucleation behavior plays a pivotal role in alleviating the dendrite formation. Herein, a practically viable route is devised by in situ crafting lithiophilic CuSe granules on the dealloyed Cu skeleton (D‐Cu@CuSe). Persuasive electrochemical analysis and systematic theoretical calculation disclose the underlying Li nucleation mechanism on the CuSe overlayer. Impressively, the D‐Cu@CuSe‐Li symmetric cell can sustain a stable plating/stripping operation over 1000 h at a high depth of discharge at 62.5%. More crucially, when paired with high‐loading sulfur cathodes, D‐Cu@CuSe‐Li||S batteries harvest advanced areal capacity and stable cycling performance even under stringent working conditions of low negative‐to‐positive (N/P) (≈2) and electrolyte‐to‐sulfur (8 μL mgs−1) ratios. Overall, a fresh perspective into rationalizing current collector design is afforded, which extends Li utilization and cycling durability in the pursuit of pragmatic Li metal anodes. [ABSTRACT FROM AUTHOR]

Witnessing compositional evolution and identifying the catalytically active moiety of electrocatalysts is of paramount importance in Li–S chemistry. Nevertheless, this field remains elusive. We report the scalable salt‐templated synthesis of Se‐vacancy‐incorporated MoSe2 architecture (SeVs‐MoSe2) and reveal the phase evolution of the defective precatalyst in working Li–S batteries. The interaction between lithium polysulfides and SeVs‐MoSe2 is probed to induce the transformation from SeVs‐MoSe2 to MoSeS. Furthermore, operando Raman spectroscopy and ex situ X‐ray diffraction measurements in combination with theoretical simulations verify that the effectual MoSeS catalyst could help promote conversion of Li2S2 to Li2S, thereby boosting the capacity performance. The Li–S battery accordingly exhibits a satisfactory rate and cycling capability even with and elevated sulfur loading and lean electrolyte conditions (7.67 mg cm−2; 4.0 μL mg−1S). This work elucidates the design strategies and catalytic mechanisms of efficient electrocatalysts bearing defects. [ABSTRACT FROM AUTHOR]

Witnessing compositional evolution and identifying the catalytically active moiety of electrocatalysts is of paramount importance in Li–S chemistry. Nevertheless, this field remains elusive. We report the scalable salt‐templated synthesis of Se‐vacancy‐incorporated MoSe2 architecture (SeVs‐MoSe2) and reveal the phase evolution of the defective precatalyst in working Li–S batteries. The interaction between lithium polysulfides and SeVs‐MoSe2 is probed to induce the transformation from SeVs‐MoSe2 to MoSeS. Furthermore, operando Raman spectroscopy and ex situ X‐ray diffraction measurements in combination with theoretical simulations verify that the effectual MoSeS catalyst could help promote conversion of Li2S2 to Li2S, thereby boosting the capacity performance. The Li–S battery accordingly exhibits a satisfactory rate and cycling capability even with and elevated sulfur loading and lean electrolyte conditions (7.67 mg cm−2; 4.0 μL mg−1S). This work elucidates the design strategies and catalytic mechanisms of efficient electrocatalysts bearing defects. [ABSTRACT FROM AUTHOR]

Designing high‐performance electrocatalysts for boosting aprotic electrochemistry is of vital importance to drive longevous Li–S batteries. Nevertheless, investigations on probing the electrocatalytic endurance and protecting the catalyst activity yet remain elusive. Here, a ternary graphene‐TiO2/TiN (G‐TiO2/TiN) heterostructure affording conformal graphene chainmail is presented as an efficient and robust electrocatalyst for expediting sulfur redox kinetics. The G‐TiO2/TiN heterostructure synergizes adsorptive TiO2, catalytic TiN, and conductive graphene armor, thus enabling abundant anchoring points for polysulfides and sustained active sites to allow smooth bi‐directional electrocatalysis. Encouragingly, in situ crafted graphene chainmail ensures favorable protection of inner TiO2/TiN to retain their catalytic robustness towards durable sulfur chemistry. As expected, sulfur cathodes mediated by ternary G‐TiO2/TiN harvest an impressive rate capability (698.8 mAh g−1 at 5.0 C), favorable cycling stability (a low decay of 0.054% per cycle within 1000 cycles), and satisfactory areal capacity under elevated loading (delivering 8.63 mAh cm−2 at a sulfur loading of 10.4 mg cm−2). The ternary heterostructure design offers an in‐depth insight into the electrocatalyst manipulation and protection toward long lifespan Li–S batteries. [ABSTRACT FROM AUTHOR]

Functionalizing carbon cathode surfaces with oxygen functional groups is an effective way to simultaneously tailor the fundamental properties and customize the electrochemical properties of aqueous Zn‐ion hybrid capacitors. In this work, the oxygen functional groups of chemically reduced graphene oxide (rGO) are systematically regulated via a series of reductants and varied experimental conductions. Carboxyl and carbonyl have been proven to significantly enhance the aqueous electrolyte wettability, Zn‐ion chemical adsorption, and pseudocapacitive redox activity by experimental study and computational analysis. The rGO cathode produced through hydrogen peroxide assisted hydrothermal reduction exhibits a specific capacitance of 277 F g−1 in 1 m ZnSO4 after optimization of surface oxygen functional groups. In addition, a quasi‐solid‐state flexible Zn‐ion hybrid capacitor (ZHC) with a polyacrylamide gel electrolyte and a high loading mass of 5.1 mg cm−2 are assembled. The as‐prepared quasi‐solid state ZHC can offer a superior areal capacitance of 1257 mF cm−2 and distinguished areal energy density of 342 µW h cm−2. The significant enhancement of redox activity and Zn‐ion storage capability by regulating the oxygen functional groups can shed light on the promotion of electrochemical charge storage properties even beyond protic electrolyte systems. [ABSTRACT FROM AUTHOR]

The rational design of electrocatalyst has readily stimulated a burgeoning interest in expediting polysulfide conversion and hence essentially restricting the "shuttle effect" in Li–S systems. Nevertheless, seldom efforts have been devoted to probing the dual‐directional polysulfide electrocatalysis to date. Herein, a CoFe alloy decorated mesoporous carbon sphere (CoFe‐MCS) serving as a promising mediator for Li–S batteries is reported. Such bimetallic alloying boosts dual‐directional electrocatalytic activity toward effective polysulfide conversion throughout detailed electroanalytic characterization, theoretical calculation, and operando instrumental probing. Accordingly, the S@CoFe‐MCS cathode harvests a stable cycling with a low capacity decay rate of 0.062% per cycle over 500 cycles at 2.0 C. More encouragingly, benefiting from the optimized redox kinetics and delicate grid architecture, printable S@CoFe‐MCS cathode achieves an excellent rate performance at a sulfur loading of 4.0 mg cm−2 and advanced areal capacity of 6.0 mAh cm−2 at 7.7 mg cm−2. This work explores non‐precious metal alloy electrocatalysts in printable cathodes toward dual‐directional polysulfide conversion, holding great potential in the pursuit of Li–S commercialization. [ABSTRACT FROM AUTHOR]

Carbonaceous materials have emerged as promising anode candidates for potassium‐ion batteries (PIBs) due to overwhelming advantages including cost‐effectiveness and wide availability of materials. However, further development in this realm is handicapped by the deficiency in their in‐target and large‐scale synthesis, as well as their low specific capacity and huge volume expansion. Herein the precise and scalable synthesis of N/S dual‐doped graphitic hollow architectures (NSG) via direct plasma enhanced chemical vapor deposition is reported. Thus‐fabricated NSG affording uniform nitrogen/sulfur co‐doping, possesses ample potassiophilic surface moieties, effective electron/ion‐transport pathways, and high structural stability, which bestow it with high rate capability (≈100 mAh g−1 at 20 A g−1) and a prolonged cycle life (a capacity retention rate of 90.2% at 5 A g−1 after 5000 cycles), important steps toward high‐performance K‐ion storage. The enhanced kinetics of the NSG anode are systematically probed by theoretical simulations combined with operando Raman spectroscopy, ex situ X‐ray photoelectron spectroscopy, and galvanostatic intermittent titration technique measurements. In further contexts, printed NSG electrodes with tunable mass loading (1.84, 3.64, and 5.65 mg cm−2) are realized to showcase high areal capacities. This study demonstrates the construction of a printable carbon‐based PIB anode, that holds great promise for next‐generation grid‐scale PIB applications. [ABSTRACT FROM AUTHOR]

[Display omitted] • The hybrid 2D/1D N -G/CNTs heterostructures with hierarchically porous architectures are simply fabricated. • DFT simulations reveal that the N -G/CNTs affords abundant active-N sites for O 2 adsorption and activation due to the efficient inter-molecular electron transfer between layers. • The optimal N -G/CNTs-900-based Zn-air battery exhibit a higher power density than that of Pt/C. Heteroatom-doped carbon-based materials have been deemed as highly efficient electrocatalysts for cathodic oxygen reduction reaction (ORR) in the sustainable energy conversion technologies. However, the limited active sites caused by the aggregation of carbon layers ineluctably hinder the mass transfer, thereby generating insufficient ORR performance. Herein, we offer a rational and facile method to manufacture a hybrid heterostructure of N -doped graphene and carbon nanotubes at the pyrolysis temperature of 900 °C (N -G/CNTs-900), which exhibits a better ORR activity than most of reported carbon-based ORR electrocatalysts, and comparable to that of Pt/C. Thus-fabricated N -G/CNTs-900 features hierarchically porous architecture, high specific surface area, abundant defects, and high active N content, and what's more, it also affords active sites for oxygen activation and subsequent 4e− reduction processes due to the hetero-interlayer charge transfer and the electron accumulations of the carbon atoms on the surface layer by theoretical calculations. Compared with commercial Pt/C, N -G/CNTs-900-based Zn-air battery presents a higher peak power density (133.60 mW/cm2) and a larger specific capacity (707 mAh/g Zn). This work provides a novel idea to design the high-efficiency and long-term durability ORR catalyst, which is benefit for boosting the commercial applications of metal-free carbon-based materials in the renewable energy conversion devices. [ABSTRACT FROM AUTHOR]

Hierarchical metal nanostructures which exhibit an open structure and a high density of twin defects accessible to reactants hold great promise in catalysis. Here, we report a facile synthesis of Pt–Cu hierarchical quasi great dodecahedrons (HQGDs) which present 5-fold symmetry and are composed of multiple ordered branched units with a frame structure. HQGDs evolve from icosahedral seeds with multiple {111} twin planes, followed by the growth of higher-order branches. Owing to the unique frame structure associated with multiple twin defects, HQGDs showed much higher HER catalytic activity and better durability relative to commercial Pt/C. [ABSTRACT FROM AUTHOR]

The elimination of wrinkles has become a research hotspot in the realm of the chemical vapor deposition growth of graphene, and there have been reliable routes developed for the scenario of catalytic synthesis on metals. Nonetheless, the transfer‐free growth of graphene over insulating substrates affording ultra‐flatness remains a puzzle. Here, the authors report the direct preparation of ultra‐flat graphene on an economical quartz glass substrate at a wafer level, without any wrinkles and metallic impurities, is reported. Density functional theory calculations are employed to establish that graphene adlayer is prone to generate in the presence of textured particulates. In parallel, a critical temperature regime (1443–1453 K), is identified within which graphene adlayer‐restrained forming and substrate in‐situ flattening could simultaneously occur. The thus‐obtained graphene enables the atomically smooth growth of a GaN film with (001) single‐crystallinity over the amorphous substrate. This technique is particularly attractive in the context of cost‐effective integration of emerging III‐nitrides toward exciting applications. [ABSTRACT FROM AUTHOR]

Co‐intercalation reactions make graphite a feasible anode in Ca ion batteries, yet the correlation between Ca ion intercalation behaviors and electrolyte structure remains unclear. This study, for the first time, elucidates the pivotal role of anions in modulating the Ca ion solvation structures and their subsequent intercalation into graphite. Specifically, the electrostatic interactions between Ca ion and anions govern the configurations of solvated‐Ca‐ion in dimethylacetamide‐based electrolytes and graphite intercalation compounds. Among the anions considered (BH4−, ClO4−, TFSI− and [B(hfip)4]−), the coordination of four solvent molecules per Ca ion (CN=4) leads to the highest reversible capacities and the fastest reaction kinetics in graphite. Our study illuminates the origins of the distinct Ca ion intercalation behaviors across various anion‐modulated electrolytes, employing a blend of experimental and theoretical approaches. Importantly, the practical viability of graphite anodes in Ca‐ion full cells is confirmed, showing significant promise for advanced energy storage systems. [ABSTRACT FROM AUTHOR]

Co‐intercalation reactions make graphite a feasible anode in Ca ion batteries, yet the correlation between Ca ion intercalation behaviors and electrolyte structure remains unclear. This study, for the first time, elucidates the pivotal role of anions in modulating the Ca ion solvation structures and their subsequent intercalation into graphite. Specifically, the electrostatic interactions between Ca ion and anions govern the configurations of solvated‐Ca‐ion in dimethylacetamide‐based electrolytes and graphite intercalation compounds. Among the anions considered (BH4−, ClO4−, TFSI− and [B(hfip)4]−), the coordination of four solvent molecules per Ca ion (CN=4) leads to the highest reversible capacities and the fastest reaction kinetics in graphite. Our study illuminates the origins of the distinct Ca ion intercalation behaviors across various anion‐modulated electrolytes, employing a blend of experimental and theoretical approaches. Importantly, the practical viability of graphite anodes in Ca‐ion full cells is confirmed, showing significant promise for advanced energy storage systems. [ABSTRACT FROM AUTHOR]

Electrochemical reduction of nitrate (NO3RR) holds great promise for environmentally friendly ammonia production. Tandem catalysis is a promising strategy for boosting the NO3RR and inhibiting side effects, but it is still challenged by lacking well‐designed catalysts to drive this catalytic process. Herein, the study develops the CuCo branched nanowires (CuCo NW) catalyst, which efficiently converts NO3 − to NH3 on Co (111) and Cu (111) crystal facets through a tandem catalysis mechanism. The in situ grown CuCo NW on Cu foam demonstrates a remarkable Faraday efficiency of 90.3% at 1.0 A cm−2 and maintains stable operation for 200 h at 100 and 200 mA cm−2 in a flow reactor. Density functional theory calculations suggest that the initial absorption and subsequent deoxygenation of *NO3 on Co (111) leading to the formation of *NO2, followed by its transfer to Cu (111) and further conversion to *NH3, establish an optimal pathway by managing rate‐determining steps on individual surfaces for NO3RR. To showcase the practical application of the catalyst, the study further develops a scaling‐up prototype reactor for continuous ammonia production, realizing the gram‐level yield rate of 1474.09 mg h−1 and Faraday efficiency of 91.26% at practical‐level 20.0 A. [ABSTRACT FROM AUTHOR]

[Display omitted] The development of a full-spectrum responsive photocatalytic germicide with excellent charge separation efficiency to harvest high antimicrobial efficacy is a key goal yet a challenging conundrum. Herein, graphitic carbon nitride nanosheet (PCNS)/Ti 3 C 2 T x MXene/TiO 2 (PMT) Z-scheme heterojunctions with robust interface contact were crafted by in situ interfacial engineering. The strong internal electrical field (IEF) from PCNS to TiO 2 , evinced by the Kelvin Probe Force Microscopy (KPFM) characterization, can obtain high charge separation efficiency with 73.99%, compared to Schottky junction PCNS/Ti 3 C 2 T x (PM, 32.88%) and PCNS (17.70%). The Ti 3 C 2 T x component can not only serve as a transfer pathway to accelerate the recombination of photoexcited electrons of TiO 2 and holes of PCNS under the Ultraviolet–visible (UV–vis) light irradiation, but also replenish the photogenic electron concentrations to semiconductors in the near-infrared (NIR) light illumination. Meanwhile, the increased temperature due to the localized surface plasmon resonance (LSPR) can further boost the electronic activity to the generation of reactive oxygen species (ROS). Taken together, the PMT performs a high disinfection efficiency up to 99.40% under full solar spectrum illumination, 3.88 and 9.75 times higher than PCNS and TiO 2 , respectively, surpassing many reported Z-scheme heterojunctions. This work offers guidance for the design of Z-scheme heterojunction with the implanting of plasmons to secure excellent full-spectrum responsive photocatalytic sterilization performance. [ABSTRACT FROM AUTHOR]

[Display omitted] • Synergistic effect of carbon edges and dopants towards ORR was predicted by DFT. • Well-designed N -GNRs contain both heteroatom-doping and abundant edge sites. • Best ORR property was obtained for N -GNRs compared to other control samples. • The synergistic effect was again demonstrated by experimental facts. Decoration with alien atoms and increasing the edge content are two valid ways to activate the oxygen reduction reaction (ORR) property of nanocarbons. To further enhance their intrinsic activity and explore the underlying ORR mechanism, graphene nanoribbons (GNRs) were selected as an ideal catalyst model. Theoretical simulations have predicted that with the synergistic effect between heteroatom-doping and edge sites, the ORR activity can be significantly improved. Inspired by this, N -GNRs were synthesized via the oxidative unzipping of CNTs followed by nitrogen incorporation with urea. Ample edges and nitrogen doping sites were detected by high-resolution transmission electron microscopy and X-ray photoelectron spectroscopy, respectively. As a result, N -GNRs exhibited remarkably higher ORR properties in terms of onset and half-wave potentials, Tafel slopes, electron transfer number and methanol tolerance than either GNRs, the control sample without doping, or N -CNTs, the control sample without abundant edges, simply clarifying the significance of synergy between dopants and edges. Thus, this work provides a simple but efficient strategy to fabricate high-performance oxygen reduction catalysts. [ABSTRACT FROM AUTHOR]

A series of V O -tunable NiFe-(oxy)hydroxides deposited on nickel foams (V O -NiFe/NF) were controllably manipulated, their electrochemical OER performance exhibited a volcano-type relationship with the percentage of V O , and positive relativity with the Ni3+/Ni2+ ratio. [Display omitted] NiFe-(oxy)hydroxides are the most active transition metal oxide electrocatalysts for oxygen evolution reaction (OER) under the alkaline media. Herein, we controllably manipulated oxygen vacancy (V O)-tunable NiFe-(oxy) hydroxides that their OER performances possessed a volcano-type relationship with V O concentration, positively-correlated with Ni3+/Ni2+ ratio. Theoretical simulations further unearthed the enhanced activation and dissociation of H 2 O by the inserting of V O. As a result, the optimal sample featuring the Ni3+/Ni2+ ratio of 30.3 % and V O of 23.8 % exhibited the overpotential of 243 mV at the current density of 100 mA cm–2, simultaneously lasting 120 h durability without any attenuation, exceding the most reported NiFe-(oxy)hydroxides. This work offers an innovative view to understand the OER performance using hypervalent Ni ratio induced by V O defects. [ABSTRACT FROM AUTHOR]

Potassium‐ion hybrid capacitors (KICs) reconciling the advantages of batteries and supercapacitors have stimulated growing attention for practical energy storage because of the high abundance and low cost of potassium sources. Nevertheless, daunting challenge remains for developing high‐performance potassium accommodation materials due to the large radius of potassium ions. Molybdenum diselenide (MoSe2) has recently been recognized as a promising anode material for potassium‐ion batteries, achieving high capacity and favorable cycling stability. However, KICs based on MoSe2 are scarcely demonstrated by far. Herein, a diatomite‐templated synthetic strategy is devised to fabricate nitrogen‐doped MoSe2/graphene (N‐MoSe2/G) composites with favorable pseudocapacitive potassium storage targeting a superior anode material for KICs. Benefiting from the unique biomorphic structure, high electron/K‐ion conductivity, enriched active sites, and the conspicuous pseudocapacitive effect of N‐MoSe2/G, thus‐derived KIC full‐cell manifests high energy/power densities (maximum 119 Wh kg−1/7212 W kg−1), outperforming those of recently reported KIC counterparts. Furthermore, the potassium storage mechanism of N‐MoSe2/G composite is systematically explored with the aid of first‐principles calculations in combination of in situ X‐ray diffraction and ex situ Raman spectroscopy/transmission electron microscopy/X‐ray photoelectron spectroscopy. [ABSTRACT FROM AUTHOR]

The single-layer dimetal oxides (MOenes) are recently predicted two-dimensional materials derived from the widely investigated MXenes. To develop high-performance hydrogen evolution reaction (HER) electro-catalysts that beyond oxygen-terminated MXenes, we theoretically proposed the oxygen-terminated V 2 O MOenes (2D V 2 O 3) and explored their potential applications as HER electro-catalysts. Through the first-principles calculations, both the 1T and 2H phases of 2D V 2 O 3 are confirmed to be structurally stable and electrically conductive. The simulations on catalytic performance and reaction mechanism on HER indicate that 2D V 2 O 3 is highly active at a low hydrogen coverage of 18.75 %, with negligible activation barrier following the Volmer-Heyrovsky mechanism. When comparing with the Ti-based and V-based MXenes, the 2D V 2 O 3 takes advantages in higher HER catalytic activity and stability of the surface termination. Moreover, the 2D V 2 O 3 is expected to be experimentally obtained by exfoliation method. [Display omitted] • Different phases of O-terminated V 2 O MOene are computationally proposed. • 2D V 2 O 3 exhibits superior HER electro-catalytic activity at low coverage of 18.75 %. • HER activation barriers are less than 0.005 eV along the Volmer-Heyrovsky mechanism. • 2D V 2 O 3 shows higher stability and activity than the V-based MXenes in HER catalysis. • 2D V 2 O 3 is expected to be experimentally obtained by exfoliation method. [ABSTRACT FROM AUTHOR]

This article provides an insightful understanding of how the surface property of N, S-co doped graphene can be modulated by the encapsulated Co 8 FeS 8 , resulting in easier OH desorption on the doped graphene surface for efficient alkaline oxygen reduction reaction. Particularly, the constructed interface for N, S-co doped graphene encapsulating Co 8 FeS 8 could evidently raise the catalytic activity through slightly positively-charged C active site, thus simultaneously enhancing electronic conductivity. [Display omitted] • An encapsulated catalyst of Co 8 FeS 8 @NSG has been successfully synthesized. • Surface property of the doped graphene can be modulated by Co 8 FeS 8. • The Co 8 FeS 8 @NSG exhibited superior catalytic activity for oxygen reduction electrocatalysis. • Greatly promoted electron transfer was achieved from the cobalt-rich sulfides to the doped graphene. • The enhanced performance was further unveiled by density functional theory calculations. Similar to proton exchange membrane fuel cell, anion-exchange membrane fuel cell is also a significant energy conversion device for achieving the utilization of clean hydrogen energy. However, the cathodic alkaline oxygen reduction reaction (ORR) is kinetically not favored and usually requires platinum-group metal (PGM) catalysts such as Pt/C to reduce the overpotential. The major challenge in using PGM-free catalysts for ORR is their low efficiency and poor stability, which urgently demands new concepts and strategies to address this issue. Herein, we controllably manufactured a N, S-co doped graphene encapsulating uniform cobalt-rich sulfides (Co 8 FeS 8 @NSG) by a universal synthesis strategy. After encapsulation, electron transfer from the encapsulated cobalt-rich sulfides to the doped graphene was greatly promoted, which effectively optimizes the electronic structure of the doped graphene, thereby enhancing the ORR activity of the doped graphene surface. Consequently, the Co 8 FeS 8 @NSG exhibits enhanced ORR activity with a higher half-wave potential of 0.868 V (versus reversible hydrogen electrode, vs. RHE) when compared with pure NSG (0.765 V vs. RHE). Density functional theory calculations further confirm that the construction of interface for NSG encapsulating cobalt-rich sulfides could conspicuously elevate the ORR activity through slightly positively-charged C active site and thus simultaneously enhancing electronic conductivity. [ABSTRACT FROM AUTHOR]

Molybdenum trioxide (MoO3) possesses high energy density but often suffers from poor electrical conductivity and limited cycling stability when used as a sodium‐ion battery (SIB) anode. To address these issues, the construction of （Molybdenum trioxide‐Molybdenum disulfide）MoO3‐MoS2 heterostructures has proven effective in enhancing electronic conductivity, ion diffusion properties, and structural stability. Guided by the density functional theory (DFT) calculations, which predict favorable Na+ diffusion and adsorption properties, nanorod‐like MoO3‐MoS2 heterostructures are synthesized using a two‐step method. Benefiting from the synergistic effects of the heterostructure and nanosized morphology, the resulting MoO3‐MoS2 electrode exhibits outstanding rate performance (316 mA h g−1 at 10 A g−1) and long‐lasting cycling stability (286 mA h g−1 after 2300 cycles at 5 A g−1) as an SIB anode. In situ XRD measurements reveal that the ultrahigh specific capacity of MoO3‐MoS2 is attributed to the synergistic intercalation‐conversion storage of MoO3 and MoS2. In the pursuit of meeting commercialization requirements, electrodes with adjustable mass loading are also prepared using 3D printing, showcasing the high areal capacity characteristics of the SIBs. This study not only provides theoretical insights into expanding the use of heterojunction materials as SIB anodes but also demonstrates the significant potential for creating high‐energy‐density and cost‐effective SIBs. [ABSTRACT FROM AUTHOR]

Highlights: G-TiO2 was fabricated via direct CVD route by growing few-layered graphene capsules over TiO2 nanotubes. K-ion hybrid capacitors based on the G-TiO2 anode and AC cathode synergized high energy and high power density.Titanium dioxide (TiO2) has gained burgeoning attention for potassium-ion storage because of its large theoretical capacity, wide availability, and environmental benignity. Nevertheless, the inherently poor conductivity gives rise to its sluggish reaction kinetics and inferior rate capability. Here, we report the direct graphene growth over TiO2 nanotubes by virtue of chemical vapor deposition. Such conformal graphene coatings effectively enhance the conductive environment and well accommodate the volume change of TiO2 upon potassiation/depotassiation. When paired with an activated carbon cathode, the graphene-armored TiO2 nanotubes allow the potassium-ion hybrid capacitor full cells to harvest an energy/power density of 81.2 Wh kg−1/3746.6 W kg−1. We further employ in situ transmission electron microscopy and operando X-ray diffraction to probe the potassium-ion storage behavior. This work offers a viable and versatile solution to the anode design and in situ probing of potassium storage technologies that is readily promising for practical applications. [ABSTRACT FROM AUTHOR]

Constructing a near-infrared (NIR) light-responsive antibacterial material keeps a preferential goal yet a huge challenge. Herein, we controllably manufactured a sandwich architecture comprised of plasmon (Ti 3 C 2 T x MXene) and photosensitizer (PANi (Ni-phytate)) locating on wide-bandgap semiconductor (TiO 2), named as PANi/TiO 2 /Ti 3 C 2 T x (PTM), which can achieve bidirectional transfer of hot-electrons under 808 nm NIR light irradiation, significantly augmenting the carrier concentration of TiO 2 surface. The increase of hot-electron concentration not only strengthens the chemical activity through the O 2 uptake simulations by the theoretical investigations, but also elevates the photothermal conversion efficiency up to 43.3 %, which is far superior to other reported photocatalytic-photothermal system. The 808 nm NIR-activated germicide can realize 99.9 % sterilization efficacy against the Escherichia coli (E. coli) with the collaboration of photocatalytic and photothermal treatment. This work offered a brand-new idea to construct a NIR-driven antimicrobial material achieving the synergistic interaction of photocatalytic therapy and photothermal therapy. [Display omitted] • Ingenious interface design of Schottky barrier benefits the separation and transfer of hot carriers. • The PTM shows 99.9 % NIR sterilization efficiency with the collaboration of photocatalytic and photothermal treatment. • The in-situ XPS and DFT calculation reveal the reaction mechanism. • The photothermal conversion efficiency reaches up to 43.3 %. [ABSTRACT FROM AUTHOR]

The anion‐exchange membrane direct ammonia fuel cell, as a carbon‐free fuel cell type, has recently received increasing attention albeit suffering from high cost of using the platinum‐group metal oxygen reduction reaction (ORR) catalysts. To pave the development of this promising power source, the atomically dispersed transition metal‐nitrogen‐carbon (M‐N‐C) materials with low cost and high ORR performance have allured to investigate their ammonia tolerance during the ORR. Herein, it is initially deconvoluted how compositional and structural elements of FeN4 sites modulate catalyst's performance. Furthermore, ORR catalytic activities of the M‐N‐C (M = Fe, Co or Mn) and Pt/C catalysts are investigated in ammonia‐containing electrolytes, showing that M‐N‐C catalysts have better ammonia tolerance than Pt/C. Among others, the Fe‐N‐C exhibits the best ammonia tolerance with only 4 mV negative shifts of half‐wave potential, 2.7% decrease of current, and negligibly irreversible activity loss. The superior ammonia tolerance of MN4 sites to Pt (111) surface is further confirmed by density functional theory calculations. The adsorption capacity of MN4 for O2 is higher than NH3 and the bonding force between MN4 and O2 is stronger than NH3, whereas opposite adsorption capacity and bonding force trends are observed on Pt (111) surface. [ABSTRACT FROM AUTHOR]

Well-designed NiO/NiCo 2 O 4 heterostructure owning abundant interface charge transfer to enhance the electrocatalytic activity of OER, supported by density functional theory (DFT) simulations. [Display omitted] Designing high-activity electrocatalysts to enhance the slow multielectron-transfer process of the oxygen evolution reaction (OER) is of great importance for hydrogen generation. Here, we employ hydrothermal and subsequent heat-treatment strategies to acquire nanoarrays-structured NiO/NiCo 2 O 4 heterojunction anchored Ni foam (NiO/NiCo 2 O 4 /NF) as efficient materials for catalyzing the OER in an alkaline electrolyte. Density functional theory (DFT) results demonstrate that NiO/NiCo 2 O 4 /NF exhibits a smaller overpotential than those of single NiO/NF and NiCo 2 O 4 /NF owing to interface-triggered numerous interface charge transfer. Moreover, the superior metallic characteristics of NiO/NiCo 2 O 4 /NF further enhance its electrochemical activity toward OER. Specifically, NiO/NiCo 2 O 4 /NF delivered a current density of 50 mA cm−2 at an overpotential of 336 mV with a Tafel slope of 93.2 mV dec−1 for the OER, which are comparable with those of commercial RuO 2 (310 mV and 68.8 mV dec−1). Further, an overall water splitting system is preliminarily constructed via using a Pt net as cathode and NiO/NiCo 2 O 4 /NF as anode. The water electrolysis cell performs an operating voltage of 1.670 V at 20 mA cm−2, which outperform the Pt net||IrO 2 couple assembled two-electrode electrolyzer (1.725 V at 20 mA cm−2). This study proposes an efficient route to acquire multicomponent catalysts with rich interfaces for water electrolysis. [ABSTRACT FROM AUTHOR]

Silver nanoparticles (Ag NPs) are used as antimicrobial agents due to their high-efficiency, broad-spectrum disinfection activity. However, the agglomeration and stability problems caused by excessive release of silver ions (Ag+) have severely restricted their developments. Herein, a novel silver/polyethyleneimine/reduced graphene oxide (Ag/PEI/rGO) antibacterial material featuring good dispersibility and permeability was rationally designed, thus benefiting for the capture of bacteria due to the introducing of highly-cationic PEI modifier and controllable release of biocidal agents (Ag+). Compared with Ag/rGO, the Ag/PEI/rGO has excellent stability and shows a more efficient sterilization efficacy against Escherichia coli (E. coli) and Staphylococcus aureus (S. aureus) with 100% germicidal efficiency with low orders of dozens of ppm. In addition, the outstanding biocompatibility of this Ag/PEI/rGO antibacterial material endows it with promising potential in sterilization applications, which is expected to solve the infection problem caused by bacterial biofilm formation. [ABSTRACT FROM AUTHOR]

The molecular structure, electrochemistry, spectroelectrochemistry and electrocatalytic oxygen reduction reaction (ORR) features of two CoII porphyrin(2.1.2.1) complexes bearing Ph or F5Ph groups at the two meso‐positions of the macrocycle are examined. Single crystal X‐ray analysis reveal a highly bent, nonplanar macrocyclic conformation of the complex resulting in clamp‐shaped molecular structures. Cyclic voltammetry paired with UV/Vis spectroelectrochemistry in PhCN/0.1 M TBAP suggest that the first electron addition corresponds to a macrocyclic‐centered reduction while spectral changes observed during the first oxidation are consistent with a metal‐centered CoII/CoIII process. The activity of the clamp‐shaped complexes towards heterogeneous ORR in 0.1 M KOH show selectivity towards the 4e− ORR pathway giving H2O. DFT first‐principle calculations on the porphyrin catalyst indicates a lower overpotential for 4e− ORR as compared to the 2e− pathway, consistent with experimental data. [ABSTRACT FROM AUTHOR]

The molecular structure, electrochemistry, spectroelectrochemistry and electrocatalytic oxygen reduction reaction (ORR) features of two CoII porphyrin(2.1.2.1) complexes bearing Ph or F5Ph groups at the two meso‐positions of the macrocycle are examined. Single crystal X‐ray analysis reveal a highly bent, nonplanar macrocyclic conformation of the complex resulting in clamp‐shaped molecular structures. Cyclic voltammetry paired with UV/Vis spectroelectrochemistry in PhCN/0.1 M TBAP suggest that the first electron addition corresponds to a macrocyclic‐centered reduction while spectral changes observed during the first oxidation are consistent with a metal‐centered CoII/CoIII process. The activity of the clamp‐shaped complexes towards heterogeneous ORR in 0.1 M KOH show selectivity towards the 4e− ORR pathway giving H2O. DFT first‐principle calculations on the porphyrin catalyst indicates a lower overpotential for 4e− ORR as compared to the 2e− pathway, consistent with experimental data. [ABSTRACT FROM AUTHOR]

Chemical vapor deposition, direct growth, graphene, ultra-flat, wafer-scale Toward Direct Growth of Ultra-Flat Graphene (Adv. Funct. Keywords: chemical vapor deposition; direct growth; graphene; ultra-flat; wafer-scale EN chemical vapor deposition direct growth graphene ultra-flat wafer-scale 1 1 1 10/21/22 20221017 NES 221017 B Ultra-Flat Graphene b In article number 2200428, Tongbo Wei, Jingyu Sun, Zhongfan Liu, and co-workers implement direct growth of wafer-level, ultra-flat graphene without any wrinkles and metallic impurities on quartz via the inhibition of textured SiO SB I x i sb seed, identification of the critical temperature regime, and in-situ flattening of the substrate surface. [Extracted from the article]

Electroreduction of CO2 into hydrocarbons could contribute to alleviating energy crisis and global warming. However, conventional electrocatalysts usually suffer from low energetic efficiency and poor durability. Herein, atomic layers for transition-metal oxides are proposed to address these problems through offering an ultralarge fraction of active sites, high electronic conductivity, and superior structural stability. As a prototype, 1.72 and 3.51 nm thick Co3O4 layers were synthesized through a fast-heating strategy. The atomic thickness endowed Co3O4 with abundant active sites, ensuring a large CO2 adsorption amount. The increased and more dispersed charge density near Fermi level allowed for enhanced electronic conductivity. The 1.72 nm thick Co3O4 layers showed over 1.5 and 20 times higher electrocatalytic activity than 3.51 nm thick Co3O4 layers and bulk counterpart, respectively. Also, 1.72 nm thick Co3O4 layers showed formate Faradaic efficiency of over 60% in 20 h. [ABSTRACT FROM AUTHOR]

[Display omitted] • Fabricated the Zn–N bonded ZnO/NC Schottky heterojunction. • Enhanced interfacial charge transfer precision through Zn–N bonds. • Utilized NC as a carrier to boost light absorption and active site exposure. • Exploited the slow-release mechanism of Zn2+ from ZnO to hasten bacterial death. Although heterogeneous photocatalytic sterilization can avoid secondary pollution and achieve broad spectrum antibacterial effects, its low disinfection efficiency seriously hinders its development. Exploring and achieving precise electron-transfer channels in the interface of heterogeneous systems are an effective method to enhance photocatalytic sterilization. Herein, we designed a chemical Zn–N bonded nitrogen-doped porous carbon-loaded zinc oxide (ZnO/NC) Schottky heterojunction photocatalyst through oxidizing and carbonizing ZIF-8 in-situ at suitable temperatures. The Zn–N accurately facilitated the photogenerated electrons transfer from the conduction band (CB) site of ZnO to the NC surface as active site. Furthermore, the NC as carrier enhanced the light-absorption capacity (746 nm) of Schottky heterojunction and functioned as active site to promote the generation of reactive oxygen species (ROS). In addition, the slow-release effect of zinc ions (Zn2+) from ZnO contributed to the accelerated death of bacteria. As a result, under simulated sunlight conditions, the ZnO/NC-400(1 h) Schottky heterojunction demonstrated an impressive antibacterial efficiency of 99.33 % against Escherichia coli , consistently exceeding 95 % in repeated experiments. This work presents a controllable and encouraging approach for constructing heterojunction with effective antibacterial properties. [ABSTRACT FROM AUTHOR]

[Display omitted] Catalytic denitrification, a promising technology for nitrate removal, is increasingly limited by the rising price of Pd. Replacing Pd with less-expensive Ru would significantly reduce the cost; however, Ru-based catalysts have been reported to perform inconsistently in denitrification applications, making their replacement prospects unclear. Herein, the surface oxidation of Ru catalysts was confirmed to be a key factor that inhibits activity. A series of Ru-Pd catalysts containing small amounts of Pd (0.5 wt%) was developed to eliminate the Ru surface-oxide layer through the spillover of hydrogen atoms activated on the Pd promoter. Ru-Pd/Fe 3 O 4 exhibited superior catalytic activity to Ru-Pd/C and Ru-Pd/Al 2 O 3 because the reducible carrier (Fe 3 O 4) has a lower resistance to hydrogen spillover and diffusion, as determined experimentally and supported by density functional theory calculations. This study developed a method that eliminates ruthenium surface oxides in situ and restores its denitrification activity, further reducing the barrier to Ru replacing Pd in catalytic aqueous denitrification. [ABSTRACT FROM AUTHOR]

Traditional materials discovery is in 'trial-and-error' mode, leading to the issues of low-efficiency, high-cost, and unsustainability in materials design. Meanwhile, numerous experimental and computational trials accumulate enormous quantities of data with multi-dimensionality and complexity, which might bury critical 'structure–properties' rules yet unfortunately not well explored. Machine learning (ML), as a burgeoning approach in materials science, may dig out the hidden structure–properties relationship from materials bigdata, therefore, has recently garnered much attention in materials science. In this review, we try to shortly summarize recent research progress in this field, following the ML paradigm: (i) data acquisition → (ii) feature engineering → (iii) algorithm → (iv) ML model → (v) model evaluation → (vi) application. In section of application, we summarize recent work by following the 'material science tetrahedron': (i) structure and composition → (ii) property → (iii) synthesis → (iv) characterization, in order to reveal the quantitative structure–property relationship and provide inverse design countermeasures. In addition, the concurrent challenges encompassing data quality and quantity, model interpretability and generalizability, have also been discussed. This review intends to provide a preliminary overview of ML from basic algorithms to applications. [ABSTRACT FROM AUTHOR]

Chemical vapor deposition (CVD) has become a promising approach for the industrial production of graphene films with appealing controllability and uniformity. However, in the conventional hot‐wall CVD system, CVD‐derived graphene films suffer from surface contamination originating from the gas‐phase reaction during the high‐temperature growth. Shown here is that the cold‐wall CVD system is capable of suppressing the gas‐phase reaction, and achieves the superclean growth of graphene films in a controllable manner. The as‐received superclean graphene film, exhibiting improved optical and electrical properties, was proven to be an ideal candidate material used as transparent electrodes and substrate for epitaxial growth. This study provides a new promising choice for industrial production of high‐quality graphene films, and the finding about the engineering of the gas‐phase reaction, which is usually overlooked, will be instructive for future research on CVD growth of graphene. [ABSTRACT FROM AUTHOR]

Chemical vapor deposition (CVD) has become a promising approach for the industrial production of graphene films with appealing controllability and uniformity. However, in the conventional hot‐wall CVD system, CVD‐derived graphene films suffer from surface contamination originating from the gas‐phase reaction during the high‐temperature growth. Shown here is that the cold‐wall CVD system is capable of suppressing the gas‐phase reaction, and achieves the superclean growth of graphene films in a controllable manner. The as‐received superclean graphene film, exhibiting improved optical and electrical properties, was proven to be an ideal candidate material used as transparent electrodes and substrate for epitaxial growth. This study provides a new promising choice for industrial production of high‐quality graphene films, and the finding about the engineering of the gas‐phase reaction, which is usually overlooked, will be instructive for future research on CVD growth of graphene. [ABSTRACT FROM AUTHOR]

• Controlled synthesis of FNP carved nanoframes was realized in a scalable manner. • Thus-fabricated FNP held promise in the realm of energy conversion and storage. • Thus-derived FNP nanoframes functioned as efficient bifunctional electrocatalysts for overall water splitting. • All-FNP, potassium-ion-battery-driven self-powering water-splitting system was constructed. Developing high-performance and cost-effective electrode materials to advance the overall water splitting and electrochemical potassium-ion storage has thus far remains appealing yet challenging. Herein, bimetallic Fe-Ni phosphide (FNP) nanoframes harvesting three-dimensional carved frameworks have been fabricated in a scalable and controllable fashion. Thus-derived FNP nanoframes have been demonstrated as efficient bifunctional electrocatalysts for overall water splitting, comparing favorably with the benchmark performance of the IrO 2 /Pt couple. Such excellent water splitting features can be attributed to the enhanced charge transfer, enlarged active surface area, facilitated electrolyte transport and promoted gas release. Density functional theory calculations reveal that the FNP owns the lowest free energy barrier of the rate-determined step for hydrogen evolution in the alkaline media as compared to the mono-metallic Fe 2 P and Ni 2 P species. In addition, as an anode candidate, FNP possesses outstanding potassium ion storage performances, showing high specific capacity (168 mAh g−1 at 50 mA g−1) and long cycle life (83% capacity retention after 700 cycles at 200 mA g−1). As a proof-of-concept demonstration, all-FNP, KIB-based self-powering water-splitting system can further be constructed, opening up exciting opportunities for the real applications of renewable energy on a basis of as-designed multifunctional FNP architectures. [ABSTRACT FROM AUTHOR]

Highlights: G-TiO2 was fabricated via direct CVD route by growing few-layered graphene capsules over TiO2 nanotubes. K-ion hybrid capacitors based on the G-TiO2 anode and AC cathode synergized high energy and high power density. Titanium dioxide (TiO2) has gained burgeoning attention for potassium-ion storage because of its large theoretical capacity, wide availability, and environmental benignity. Nevertheless, the inherently poor conductivity gives rise to its sluggish reaction kinetics and inferior rate capability. Here, we report the direct graphene growth over TiO2 nanotubes by virtue of chemical vapor deposition. Such conformal graphene coatings effectively enhance the conductive environment and well accommodate the volume change of TiO2 upon potassiation/depotassiation. When paired with an activated carbon cathode, the graphene-armored TiO2 nanotubes allow the potassium-ion hybrid capacitor full cells to harvest an energy/power density of 81.2 Wh kg−1/3746.6 W kg−1. We further employ in situ transmission electron microscopy and operando X-ray diffraction to probe the potassium-ion storage behavior. This work offers a viable and versatile solution to the anode design and in situ probing of potassium storage technologies that is readily promising for practical applications. [ABSTRACT FROM AUTHOR]

TiO 2 /W 18 O 49 /Ti 3 C 2 T x -MXene ternary heterojunction possessed dual electron transmission channels, one is the Z-scheme mode from the W 18 O 49 and TiO 2 and the other is that electrons on the TiO 2 transferred across the Schottky-junction to the MXene. As a result, the separation efficiency of photogenerated electrons and holes can be greatly enhanced and abundant bactericidal active substances such as •O 2 – and •OH were generated to realize an improved photocatalytic sterilization of E. coli. [Display omitted] • A TiO 2 /W 18 O 49 /Ti 3 C 2 T x MXene heterojunction was fabricated via solvothermal method. • Z-scheme heterojunction and Schottky-junction coexist in the composite. • A synergistic effect in the composite boosts the sterilization performance. • The TiO 2 /W 18 O 49 /Ti 3 C 2 T x MXene possesses good biocompatibility. Construction of multiple electronic transmission channels in a photocatalytic system is in favor of boosting the charge separation to realize a high photocatalytic antibacterial property. Herein, a novel hierarchical ternary photocatalyst consisting of TiO 2 /W 18 O 49 Z-scheme heterojunction and Ti 3 C 2 T x -MXene cocatalyst was synthesized via a simple two-step solvothermal method. Dual charge transfer routes were realized in this TiO 2 /W 18 O 49 /Ti 3 C 2 T x -MXene composite. The electrons on TiO 2 can transfer either through the Z-scheme mode to combine with the holes of W 18 O 49 , or through the Schottky-junction to Ti 3 C 2 T x -MXene cocatalyst. The TiO 2 /W 18 O 49 /Ti 3 C 2 T x -MXene composite maintained high photooxidation-reduction capacity and possessed fast charge separation behavior. As a result, the TiO 2 /W 18 O 49 /Ti 3 C 2 T x -MXene heterojunction had a high photocatalytic bactericidal rate of 93.7% for Escherichia coli (E. coil) under light (λ ≥ 365 nm, 6 h), which was 3.3, 5.5, 3.1 and 2.9 times that of MXene (28.6%), TiO 2 (17.0%), W 18 O 49 (30.0%) and TiO 2 /MXene (32.8%), respectively. In addition, the ternary heterojunction illustrated good biocompatibility. This work provides a simple method of constructing multiple electronic transmission channels for high bactericidal performance and proves the effectiveness of photocatalytic materials in the biological field. [ABSTRACT FROM AUTHOR]

Employing a suitable cocatalyst is very important to improve photocatalytic H 2 evolution activity. Herein, two plasmonic cocatalysts, Au nanoparticles and TiN nanoparticles were in-situ coupled over the g-C 3 N 4 nanotube to form a ternary 0D/0D/1D Au/TiN/g-C 3 N 4 composite via a successive thermal polycondensation and chemical reduction method. The g-C 3 N 4 nanotube acted as a support for the growth of Au and TiN nanoparticles, leading to intimate contact between g-C 3 N 4 nanotube with Au nanoparticles and TiN nanoparticles. As a result, multiple interfaces and dual-junctions of Au/g-C 3 N 4 Schottky-junction and TiN/g-C 3 N 4 ohmic-junction were constructed, which helped to promote the charged carriers' separation and enhanced the photocatalytic performance. Furthermore, loading plasmonic cocatalysts of Au nanoparticles and TiN nanoparticles can enhance the light absorption capacity. Consequently, the Au/TiN/g-C 3 N 4 composite exhibited significantly enhanced photocatalytic H 2 evolution activity (596 μmol g−1 h−1) compared to g-C 3 N 4 or binary composites of Au/g-C 3 N 4 and TiN/g-C 3 N 4. This work highlights the significant role of cocatalysts in photocatalysis. [Display omitted] • LSPR enhanced 0D/0D/1D Au/TiN/g-C 3 N 4 composite was prepared. • Au and TiN dual plasmonic cocatalysts provided more active sites. • Double junctions were formed to offer dual electron transfer route. • Au/TiN/g-C 3 N 4 composite exhibited enhanced photocatalytic H 2 evolution activity. [ABSTRACT FROM AUTHOR]

The integration of boron doping with high curvature surface is achieved in bismuth catalyst for photoelectrochemical nitrogen fixation. Boron doping in Bi catalyst reduces the energy barrier of the potential-determining step of N 2 reduction and high curvature structure facilitates the N 2 adsorption. The designed catalyst displays NH 3 yield rate of 29.2 mg NH3 g cat. −1 h−1 and Faradaic efficiency of 8.3 % when used as cathode in photoelectrochemical nitrogen fixation. • Integration of B doping with high curvature structure is achieved in Bi catalyst by reducing layered BiOBr nanosheets. • B doping in Bi catalyst reduces the energy barrier of the potential-determining step of nitrogen reduction. • High curvature Bi surface facilitates N2 adsorption. • B-doped Bi nanoroll catalyst displays substantially enhanced photoelectrochemical nitrogen fixation performance. Photoelectrochemical (PEC) nitrogen reduction reaction (NRR), which produces ammonia under ambient conditions by combining the merits of electrocatalysis and photocatalysis, represents an attractive prospect for nitrogen fixation. Limited by the choice of suitable p-type semiconductor, PEC nitrogen fixation should be preferentially achieved by cathodic NRR integrated with photoanode rather than direct photocathodic NRR. Even in such an approach, it still remains elusive how to design catalytically active sites on the dark cathode toward high activity and selectivity in PEC NRR. Herein, we report a new strategy for tailoring cathodic bismuth (Bi) sites with boron (B) doping and rolling curvature. The B doping in Bi matrix greatly reduces the energy barrier of the potential-determining step of N 2 → *NNH in NRR while the high curvature surface on nanorolls facilitates the adsorption of N 2. The integration of B doping and rolling curvature in a single cathodic catalyst boosts PEC NRR performance when combined with TiO 2 nanorods array as photoanode to harvest light and provide photo-generated electrons. Such a PEC system offers an ammonia yield rate of 29.2 mg NH3 g cat. −1 h−1 and Faradaic efficiency of 8.3 % at a bias of 0.48 V versus RHE in nitrogen fixation. This work provides a guideline for the rational design of highly active and selective metallic catalyst in PEC NRR. [ABSTRACT FROM AUTHOR]