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Single‐atom catalysts (SACs) are widely studied in various chemical transformations due to their high catalytic activity and atom utilization. However, modulating the catalytic performance of catalysts by adjusting the microenvironment remains a great challenge. In this paper, a novel master‐double guest vulcanization‐assisted strategy is reported for synthesizing Fe single‐atom catalysts on N,S codoped porous hollow leaf carbon (FeSA/N,S‐PHLC) with highly exposed FeN3SOH sites. Fe(mIm) (guest I) is loaded on the surface of ZIF‐L (host) and then trithiocyanuric acid (TCA, guest II) is bonded with Fe(mIm), and the resulting ZIF‐L@Fe(mIm)@TCA precursors can be converted to FeSA/N,S‐PHLC with controllable structures. In addition, XPS analysis yield an increase in pyridine N content in FeSA/N,S‐PHLC compared to FeSA/N‐PHLC. It can be demonstrated by theoretical calculations that the N,S‐coordinated axially hydroxy‐coordinated asymmetric Fe centers synergistically with the abundance of pyridinic nitrogen facilitate the adsorption and desorption of oxygen intermediates, and the 3d orbitals of the Fe active centers can be optimized. The prepared FeSA/N,S‐PHLC catalyst has a half‐wave potential (E1/2) of 0.91 V under alkaline conditions, and E1/2 = 0.75 V under acidic conditions. It shows excellent cycle stability (882 h) and power density (217 mW cm−2) in the assembly of zinc–air battery (ZABs) devices. [ABSTRACT FROM AUTHOR]

It is a great challenge to induce the formation of the RuP4 phase and realize the construction of a metal‐rich phase/phosphorus‐rich phase‐ruthenium phosphide heterostructure by directional regulation of the proportion of P and metal atoms. The ultra‐high conductivity of Ru2P and the excellent ability of V‐doped RuP4 to absorb/desorb H* are confirmed by density functional theory (DFT) calculations, which laid a theoretical foundation for the construction of a unique Ru2P/V‐RuP4 structure to accelerate HER reaction kinetics. This work innovatively uses the V‐doping strategy to induce the formation of RuP4 phase with high intrinsic activity, and finally construct V‐RuxPy nanosheets with rich Ru/Ru2P/V‐RuP4 heterostructures. Thanks to the rich Ru/Ru2P/V‐RuP4 heterostructure and the optimization of V dopants, the V‐RuxPy catalyst only needs 180 mV to obtain an industrial‐grade current density of 1 A cm−2. In summary, this work provides a new idea for the design and performance optimization of ruthenium‐based catalysts. [ABSTRACT FROM AUTHOR]

For the pursuit of high energy supercapacitors, the development of high performance pseudocapacitance or battery-type negative electrode material is urgently needed to make up for the capacity shortage of commercial electric double layer capacitor (EDLC) type materials. Herein, a porous and defect-rich FexBi2−xS3 solid solution structure is firstly constructed by employing Fe-doped Bi2O2CO3 porous nanosheets as a precursor, which presents dramatically increased energy storage performance than Bi2S3 and FeS2 phase. For the optimized FexBi2−xS3 solid solution (FeBiS-60%), the Fe solute is free and random dispersed in Bi2S3 framework, which can effectively modulate the electronic structure of Bi element and introduce rich-defect due to the existence of Fe(II). Meanwhile, the FeBiS-60%, constructed by pore nanosheets that are assembled by self-supported basic nanorod units, presents rich mesoporous channels for fast mass transfer and abundant active sites for promoting capacity performance. Therefore, a high capacitance of 832.8 F·g−1 at a current density of 1 A·g−1 is achieved by the FeBiS-60% electrode. Furthermore, a fabricated Ni3S2@Co3S4 (NCS)//FeBiS-60% hybrid supercapacitor device delivers an outstanding energy density of 85.33 Wh·kg−1 at the power density of 0.799 kW·kg−1, and ultra-long lifespan of remaining 86.7% initial capacitance after 8700 cycles. [ABSTRACT FROM AUTHOR]

Ru dopants enhanced electrocatalytic performance by optimizing the electronic configuration, but how to efficiently dope Ru and introduce strain effect is a challenge. In this work, Vb12 is used to introduce the CN layer into phosphides and effectively increase the doping amount of Ru. Notably, Ru dopants induce Ni2P to produce a tensile strain of 0.172%, effectively optimizing the electronic configuration of Ru-Ni2P. Obviously, Ni with more positive charges acts as the UOR active site, and the optimized Ru acts as the HER active site, synergistically promoting urea-assisted total water decomposition. Surprisingly, the Ru-Ni2P@CN catalyst only required a potential of 1.412 V to drive 1 A cm−2 for urea-assisted water splitting. With the help of Vb12, abundant Ru dopants, and tensile strain were successfully introduced into the phosphide electrode, which provided a new idea for optimizing the performance of the phosphide electrode. [ABSTRACT FROM AUTHOR]

Early detection is critical to achieving improved treatment outcomes for child patients with congenital heart diseases (CHDs). Therefore, developing effective CHD detection techniques using low-cost and non-invasive pediatric electrocardiogram are highly desirable. We propose a deep learning approach for CHD detection, CHDdECG, which automatically extracts features from pediatric electrocardiogram and wavelet transformation characteristics, and integrates them with key human-concept features. Developed on 65,869 cases, CHDdECG achieved ROC-AUC of 0.915 and specificity of 0.881 on a real-world test set covering 12,000 cases. Additionally, on two external test sets with 7137 and 8121 cases, the overall ROC-AUC were 0.917 and 0.907 while specificities were 0.937 and 0.907. Notably, CHDdECG surpassed cardiologists in CHD detection performance comparison, and feature importance scores suggested greater influence of automatically extracted electrocardiogram features on CHD detection compared with human-concept features, implying that CHDdECG may grasp some knowledge beyond human cognition. Our study directly impacts CHD detection with pediatric electrocardiogram and demonstrates the potential of pediatric electrocardiogram for broader benefits. Congenital heart disease is life threatening, and its screening is complex and costly. Here, authors use AI to detect the disease based on pediatric electrocardiogram, suggesting superior performance over cardiologists. [ABSTRACT FROM AUTHOR]

The hydrogen energy generated by the electrocatalytic water splitting reaction has been established as a renewable and clean energy carrier with ultra‐high energy density, which can well make up for shortcomings of conventional renewable energy sources, such as geographical limitations, climatic dependence, and energy wastage. Notably, the introduction of electrocatalysts can enhance the efficiency of the water splitting process to generate hydrogen. Particularly, the heterostructure electrocatalysts constructed by coupling multiple components (or phases) have emerged as the most promising option for water splitting due to the well‐known electronic and synergistic effects. The existing reviews on interface engineering for electrocatalyst design mostly focus on the relationship between the heterostructures and specific electrocatalytic reactions. However, a comprehensive overview of the integration of model building, directional synthesis, and electrocatalytic mechanism has been rarely reported. To this end, in this review, the development of heterostructure catalysts is systematically introduced from the perspective of interface classification, interface growth and synthesis, and regulation of electrocatalytic performance based on the interfacial microenvironment (bonding, electronic configuration, lattice strain, etc.), thereby offering useful insights on the design and construction of interfacial models. Besides, combined with the current development and applications of interface engineering strategies, the challenges of future heterostructure catalysts are discussed and relevant solutions are proposed. Overall, this review can serve as a useful theoretical reference for the integration of interfacial model building, directional synthesis, and electrocatalytic mechanism, which can further promote the development of hydrogen production technologies with low energy consumption and high yield. [ABSTRACT FROM AUTHOR]

The interface engineering strategy is deemed to be a direct approach for boosting the water splitting activity of materials, but it is still a challenge to achieve both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) activities exceeding those of precious-metal catalysts. Herein, a tunable photodeposition method was utilized for the construction of Ru@FeCoP with rich Ru/FeCoP heterointerfaces. Strikingly, the η100 value of Ru@FeCoP was only 0.0741 V for the HER and 0.314 V for OER, which was reduced by 63.8% and 55.2% compared to Pt/C and RuO2 benchmarks, respectively. The mechanism investigation revealed that Ru at the Ru/FeCoP heterointerfaces not only offers highly active sites for HER but also pulls electrons from FeCoP, which facilitates the generation of Fe and Co with high valency, thereby increasing the OER activity. This work overcomes the problem of low water-splitting efficiency of precious metals by constructing a metal/phosphide heterostructure to drive a dual-active site mechanism and provides an effective route for the preparation of high-performance water-dissociation electrocatalysts. [ABSTRACT FROM AUTHOR]

Currently, the construction of heterostructures to optimize electrocatalytic activities is a hot research topic, since there is still a certain gap between the electrocatalytic properties of these heterostructures and that of Pt/C. With this in mind, we utilized in‐situ vapor‐phase phosphorization‐sulfurization to obtain the CoP3/MoS2−Co0.75Mo3S3.75 (CoP/CoMoS, for short) heterostructure on carbon cloth (CC), which exhibits Pt‐like electrocatalytic performance and excellent stability in acid electrolyte. Activated by CoP3 active phase, the electronic configuration of CoMoS and the adsorption energy of H* (▵GH*) are greatly optimized. Meanwhile, the rapid oxidation of CoMoS phase can be effectively avoided under the protection of CoP3 layer. This work provides a reference for the design of heterostructures and their mechanism of action in electrocatalysis. [ABSTRACT FROM AUTHOR]

Transition metal phosphide is regarded as one of the most promising candidates to replace noble‐metal hydrogen evolution reaction (HER) electrocatalysts. Nevertheless, the controllable design and synthesis of transition metal phosphide electrocatalysts with efficient and stable electrochemical performance are still very challenging. Herein, a novel hierarchical HER electrocatalyst consisting of three‐dimensional (3D) coral‐like Mn‐doped Co2P@an intermediate layer of Ni2P generated in situ by phosphorization on Ni foam (MnCoP/NiP/NF) is reported. Notably, both the incorporation of Mn and introduction of the Ni2P interlayer promote Co atoms to carry more electrons, which is beneficial to reduce the force of the Co−H bond and optimize the adsorption energy of hydrogen intermediate (|ΔGH*|), thereby making MnCoP/NiP/NF exhibit outstanding HER performance with onset overpotential and Tafel slope as low as 31.2 mV and 61 mV dec−1, respectively, in 1 m KOH electrolyte. [ABSTRACT FROM AUTHOR]

Rational construction of high‐efficiency and low‐cost catalysts is one of the most promising ways to produce hydrogen but remains a huge challenge. Herein, interface engineering and heteroatom doping were used to synthesize V‐doped sulfide/phosphide heterostructures on nickel foam (V‐Ni3S2/NixPy/NF) by phosphating treatment at low temperature. The incorporation of V can adjust the electronic structure of Ni3S2, expose more active sites, and protect the 3D structure of Ni foam from damage. Meanwhile, the heterogeneous interface formed between Ni3S2 and NixPy can provide abundant active sites and accelerate electron transfer. As a result, the V‐Ni3S2/NixPy/NF nanosheet catalyst exhibits outstanding activity in the hydrogen evolution reaction (HER) with an extremely low overpotential of 90 mV at a current density of 10 mA cm−2 and stable durability in alkaline solution, which exceeds those most of the previously reported Ni‐based materials. This work shows that rational design by interfacial engineering and metal‐atom incorporation has a significant influence for efficient hydrogen evolution. [ABSTRACT FROM AUTHOR]

A heterogeneous structure formed by coupling two or more phases can reinforce the activity of active sites and expedite electron transfer, which is conducive to boosting its electrocatalytic activity. Herein, we designed nickel foam supported (NiCo2)Se@Ni(OH)2 (NCS@NH) heterojunction nanosheets by a two-step method. First of all, the NiCo2S4@Ni(OH)2 (NiCo2S4@NH) nanosheets coated on nickel foam were acquired via a hydrothermal method. In the selenization treatment that followed, NiCo2S4@NH was converted into NCS@NH heterogeneous nanosheets in which the selenide nanoparticles decorated on the surface of the Ni(OH)2 nanosheets formed heterojunction interfaces, and the heterogeneous structure could accelerate electron transfer, thus improving the catalytic activity. The Ni(OH)2 nanosheets can adequately contact the electrolyte and promote the decomposition of water. Meanwhile, the thickness of the Ni(OH)2 nanosheets gradually decreases with the increase of Co doping (1.5–2.5 mmol), consequently affecting the HER properties. Notably, when the amount of Co salt added is 2 mmol, NCS@NH exhibited superior HER properties (with a voltage of 253 mV at 100 mA cm−2) and excellent stability for 24 h. [ABSTRACT FROM AUTHOR]

The catalytic properties of non-noble metal catalysts are not comparable to those of noble metal catalysts, such as Pt and Ru, on account of the catalytic thresholds of these non-noble metal catalysts. In order to solve this problem, an efficient P, W-MoS2/NiSP/NF catalyst was rationally designed through heteroatom (P and W) doping and heterostructure construction. Interestingly, motivated by the synergistic incorporation of W and P, the 2H-phase MoS2 with limited edge active sites was partially converted into highly active 1T-phase MoS2 with rich defects, which basically activate the hydrogen evolution reaction (HER)-inert basal plane of MoS2 and significantly enlarge the number of active sites, ultimately endowing the well-designed P, W-MoS2/NiSP/NF catalyst with Pt-like HER performance and superior oxygen evolution reaction (OER) performance. Importantly, this work exerts a profound influence on the construction of 1T-MoS2 with defects, the design of multi-stage structures, and the achievement of Pt-like catalytic performance. [ABSTRACT FROM AUTHOR]

The introduction of metal atom or heteroatom into transition metal phosphide is an effective strategy to enhance the electrochemical activity for hydrogen evolution reaction, while the controllable synthesis and purposeful design of efficient and stable transition metal phosphide based electrocatalyst with typical structural morphology is still a big challenge. Here, we investigated the relationship among the variety of the doped metal element (Fe and Mn), the corresponding morphology and electrocatalytic performance of the obtained sample for hydrogen evolution reaction. We found that with the doping of Fe and Mn, the cylinder-like CoP has transformed into microflower-like CoP-FeP and rambutan-like CoP-MnP, respectively. Meanwhile, the obtained CoP-FeP exhibits the excellent electrocatalytic activity hydrogen evolution reaction (HER) over a wide pH range (0–14), followed by CoP-MnP and CoP, resulting from the typical nanostructure and the moderately optimized electronic structure of P and Co center. Image 1 • CoP-MP (M = Fe, Mn) nanomaterials with different morphology have been controlled synthesized. • CoP-FeP shows excellent electrochemical performance for HER over a wide pH range (0–14). • The introduction of Fe or Mn element could optimized electronic structure of Co centers and P. [ABSTRACT FROM AUTHOR]

Hydrogen evolution reaction (HER) via electrocatalysis using cost-efficient bimetallic phosphide as electrocatalyst holds a great promise for environmentally friendly energy technologies. Here we report a novel strategy to synthesize a series of CoNiP multi-shelled hollow microspheres with different ratios of Co to Ni using metal–organic framework as both the precursor and the template, and the as-obtained CoNiP-0.25 presents a pre-eminent electrocatalytic activity for the hydrogen evolution reaction (HER) in 1.0 M KOH. The CoNiP-0.25 microspheres are found to drive 20 mA cm−2 at a potential of 170 mV vs. RHE, which is 120 mV and 59 mV smaller than that of pure NiP and CoP, respectively. The outstanding HER activity of the CoNiP-0.25 microspheres can be attributed to the optimization of their electronic structure, the typical multi-shelled hollow structure and the massive exposure of the active phase bimetallic phosphide CoNiP. Moreover, the enhanced electrochemical stability of CoNiP electrocatalyst might also stem from its special structure of multi-shelled hollow microsphere, which inhibits its superficial oxidation during the catalytic process. [ABSTRACT FROM AUTHOR]

Abstract Stable, earth-abundant and efficient electrocatalysts for overall water splitting are urgently needed. In this work, we have reported the synthesis of FeNiP/NC hollow microboxes (FeNiP/NC) based bifunctional electrocatalyst via the phosphorization process using rationally designed cube-type metal-organic framework (FeNi-MOF) as both the template and carbon source. The FeNiP/NC, which were obtained by assembling the uniform FeNiP nanoparticals together through N-doped carbon, manifests outstanding catalytic performances for both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in KOH solution. Notably, FeNiP/NC displays exceptional activity when it was utilized as both anode and cathode toward overall water splitting with potential of 1.54 V at a current density of 10 mA cm−2 in alkaline electrolyte, which is much better than FeP/NC and Ni 2 P/NC electrocatalyst. More importantly, the improvement of the catalytic activities of FeNiP/NC mainly benefits from the well dispersion of FeNiP nanoparticles on the surface of carbon support, the large active surface area and the doping of N and C derived from organic ligands. In addition, the enhanced electrocatalytic performance of FeNiP/NC for OER is closely related with the in-situ formed surficial MOOH (M = Fe, Ni) active sites, which has been confirmed by X-ray photoelectron spectroscopy (XPS) analysis. Graphical abstract Image 1 Highlights • Uniform FeNiP nanoparticles assembled together through N-doped carbon based hollow microboxs have been synthesized. • FeNiP/NC was obtained using FeNi-MOF as precursor. • Hollow FeNiP/NC is a bifunctional electrocatalyst for HER and OER in alkaline media. • The MOOH (M = Fe, Ni) with high activity for OER have in-situ formed on the surface of FeNiP/NC. [ABSTRACT FROM AUTHOR]

Platinum (Pt)‐based compounds are the benchmarked catalysts for hydrogen evolution reaction (HER) but exhibit slow kinetics in alkaline environments. The *OH accumulation on Pt surface can block active sites, affecting proton reduction and water re‐adsorption. Alloying Ruthenium (Ru) with Pt sites can significantly modulate the adsorption and desorption of water dissociation intermediates. Choosing suitable supports and utilizing metal‐support interaction (MSI) is crucial for active site optimization. PtRu alloy anchored on tungsten oxide (WO3) with rich oxygen vacancies (OV) is prepared through an ultrafast microwave‐assisted approach. Benefiting from the coupling effects between alloying and MSI, PtRu/WO3‐OV exhibits exceptionally high HER activity. In 1 m KOH, 1 m KOH + seawater, and 0.5 m H2SO4, it requires ultralow overpotentials of 9, 26, and 6 mV to achieve 10 mA cm−2, respectively. The designed catalyst surpasses commercial Pt/C in mass activity and demonstrates considerable potential for intermittent energy integration. Density functional theory reveals that alloying Ru with Pt sites significantly reduces the energy barrier of dissociating *OH, modulating blockage on the surface and then promoting the overall alkaline HER process. This study offers insights into the rapid synthesis of non‐carbon supported catalysts with Pt site modulation for alkaline hydrogen generation. [ABSTRACT FROM AUTHOR]

In this work, nickel cobalt bimetallic sulfide with typical multi-shell hollow sphere structure behaved superior electrocatalytic activity towards hydrogen evolution reaction (HER), which have been prepared through a easy method included solvothermal step, calcination step and in-situ sulfurization step. The composition and structure of the obtained nickel cobalt bimetallic sulfide are controlled through adjusting the sulfurization temperature and dosage of sulfur source. The as-prepared Ni–Co-S multi-shell hollow microspheres (abbreviated as Ni-Co-S) behaves superb HER properties in alkaline medium and Ni-Co-S-340(60) performs the most superior property, in which reflected the lowest overpotential (129 mV vs. RHE) at the current density of 10 mA cm−2 and the smallest Tafel slope (96.1 mV dec−1) among all the synthesized samples. The superior electrocatalytic performance of the obtained Ni-Co-S-340(60) for HER is owing to the unique multi-shell hollow structure derived from the intrinsic porous character of Ni-Co-BTC MOF precursor in one hand. And in the other hand, introducing highly active NiCo 2 S 4 into NiS 2 would enhance its elctrocatalytic activity because of the strong interfacial effect between NiS 2 and NiCo 2 S 4. Image 1 [ABSTRACT FROM AUTHOR]

Using low cost and high efficiency non-precious bimetallic phosphosulphide as electrocatalyst for hydrogen evolution reaction (HER) is not only convenient but also environment-friendly for industrial production. Therefore, we propose a simple and efficient method to prepare a series of Cu-doped bimetallic phosphosulphide nanosheet arrays on nickel foam (CuNiS@Ni 2 P/NF). The CuNiS@Ni 2 P/NF exhibits the superior HER performance with appropriate doping amount of Cu. It just needs a potential of 144 mV to obtain the current density of 10 mA cm−2 in 1.0 M KOH, which is smaller than that of CuNiS@Ni 2 P/NF-0.25 (206 mV) and CuNiS@Ni 2 P/NF-0.125 (219 mV). The excellent HER performance of CuNiS@Ni 2 P/NF nanosheet arrays can be ascribed to: (i) the moderate Cu-doped effectively optimized the electronic structure and morphology of the electrocatalyst; (ii) typical nanosheet arrays structures exposing more active sites; (iii) the high immanent activity excited by the multi-component synergy. • Cu-doped bimetallic phosphosulphide nanosheet arrays on Ni foam has been prepared. • The moderate amount of Cu doping could optimize the electronic structure of the product. • The typical structure and multi-component synergy contribute to the enhanced performance. [ABSTRACT FROM AUTHOR]

• The RuP 4 @CoP/Ti electrocatalyst with acacia-like structure was obtained using a facile method. • The incorporation of Ru can accelerate the charge transfer between Ru, Co, and P. • The RuP 4 @CoP/Ti possesses super activity under either acidic or alkaline solution. • The existence of Ti foil could enhance the electrical conductivity and disperse the active phases. The transition metal phosphate with lower price and rich abundance have a tendency to replace Pt-based catalytic materials for hydrogen evolution reaction (HER). Nevertheless, for transition metal phosphate based electrocatalyst, the further improvement of the electrocatalytic performance and the deep exploration of the regulation and control mechanism are still bottleneck problems. At present, we use a novel method to prepare the Ti foil supported the CoP acacia-like arrays decorated with RuP 4 nanoparticles composite (RuP 4 @CoP/Ti). The obtained RuP 4 @CoP/Ti possesses excellent electrocatalytic performance, which needs the overpotential of 66.2 mV to reach the current of density of 10 mA cm−2 and has the Tafel slope of 52.6 mV dec−1 in 0.5 M H 2 SO 4. In addition, it requires the overpotential of 36 mV to reach the current of density of 10 mA cm−2 and has Tafel slope of 54.8 mV dec−1 in 1 M KOH. Moreover, the obtained RuP 4 @CoP/Ti also presents outstanding long-term durability under either acidic or alkaline condition. The reason for such excellent properties is due to the unique acacia-like structure, the synergistic effect between CoP and RuP 4 , the existence of Ti foil and the introduction of Ru, which can optimize the electronic structure of Co and P. [ABSTRACT FROM AUTHOR]