Heterometallic Electrocatalysts Derived from High-Nuclearity Metal Clusters for Efficient Overall Water Splitting DOI

Fu-Chun Pan,

Jun Jia,

Feng Gong

et al.

ACS Nano, Journal Year: 2024, Volume and Issue: 18(8), P. 6202 - 6214

Published: Feb. 12, 2024

The development of cost-effective electrocatalysts with an optimal surface affinity for intermediates is essential sustainable hydrogen fuel production, but this remains insufficient. Here we synthesize Ni2P/MoS2-CoMo2S4@C heterometallic based on the high-nuclearity cluster {Co24(TC4A)6(MoO4)8Cl6}, in which Ni2P nanoparticles were anchored to MoS2-CoMo2S4@C nanosheets via strong interfacial interactions. Theoretical calculations revealed that introduction phases induces significant disturbances electronic configuration Ni2P/MoS2-CoMo2S4@C, resulting more relaxed d–d orbital electron transfers between metal atoms. Moreover, continuous transport was established by formation multiple heterojunction interfaces. optimized electrocatalyst exhibited ultralow overpotentials 198 and 73 mV oxygen evolution reactions, respectively, alkaline media, at 10 mA cm–2. alkali electrolyzer constructed using required a cell voltage only 1.45 V (10 cm–2) drive overall water splitting excellent long-term stability.

Language: Английский

Water electrolysis for hydrogen production: from hybrid systems to self-powered/catalyzed devices DOI
Jin‐Tao Ren, Lei Chen, Haoyu Wang

et al.

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 17(1), P. 49 - 113

Published: Nov. 7, 2023

This perspective highlights recent advancements in innovative strategies to provide valuable insights into the potential for energy-saving hydrogen production through water electrolysis.

Language: Английский

Citations

197

Defect Engineered Metal–Organic Framework with Accelerated Structural Transformation for Efficient Oxygen Evolution Reaction DOI Open Access

Jieting Ding,

Danyu Guo,

Nanshu Wang

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(43)

Published: Sept. 6, 2023

Metal-organic frameworks (MOFs) have been increasingly applied in oxygen evolution reaction (OER), and the surface of MOFs usually undergoes structural transformation to form metal oxyhydroxides serve as catalytically active sites. However, controllable regulation reconstruction process remains a great challenge. Here we report defect engineering strategy facilitate during OER with enhanced activity. Defective (denoted NiFc'x Fc1-x ) abundant unsaturated sites are constructed by mixing ligands 1,1'-ferrocene dicarboxylic acid (Fc') defective ferrocene carboxylic (Fc). series more prone be transformed compared non-defective (NiFc'). Moreover, as-formed derived from contain vacancies. NiFc'Fc grown on nickel foam exhibits excellent catalytic activity an overpotential 213 mV at current density 100 mA cm-2 , superior that undefective NiFc'. Experimental results theoretical calculations suggest vacancies adsorption oxygen-containing intermediates centers, thus significantly improving

Language: Английский

Citations

124

Nanoreactors Encapsulating Built‐in Electric Field as a “Bridge” for Li–S Batteries: Directional Migration and Rapid Conversion of Polysulfides DOI
Junhao Li, Zhengyi Wang, Kaixiang Shi

et al.

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 14(9)

Published: Dec. 27, 2023

Abstract Lithium–sulfur batteries (Li–S) are recognized as the next generation of secondary due to their satisfactory theoretical specific capacity and energy density. However, a series problems such disordered migration behavior, sluggish redox kinetics, serious shuttle effect lithium polysulfides (LiPSs) greatly limit commercial application. Herein, nanoreactors encapsulate heterostructure guarantee sulfur conversion in hosts where consists FeP with moderate adsorption ability, excellent catalytic active low work function, Fe 3 O 4 strong ability high function. This rational configuration controls direction interface built‐in electric field (BIEF) between catalyst adsorbent, realizing successive “trapping‐directional migration‐conversion” reaction mechanism species. Thanks BIEF bridge connect trapping site site, /FeP@C─S cathode delivers an ultrahigh initial 1402 mAh g −1 at 0.1 C remains more than 450 5 after 350 cycles. Even loading 5.20 mg cm −2 , it displayed 970 . provided effective strategy design high‐performance electrocatalysts for Li–S batteries.

Language: Английский

Citations

102

Regulating Hydrogen/Oxygen Species Adsorption via Built‐in Electric Field ‐Driven Electron Transfer Behavior at the Heterointerface for Efficient Water Splitting DOI
Wenjie Zhang, Lei Yang, Zhi Li

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(16)

Published: Feb. 29, 2024

Abstract Alkaline water electrolysis (AWE) plays a crucial role in the realization of hydrogen economy. The design and development efficient stable bifunctional catalysts for both evolution reaction (HER) oxygen (OER) are pivotal to achieving high‐efficiency AWE. Herein, WC 1‐x /Mo 2 C nanoparticle‐embedded carbon nanofiber (WC C@CNF) with abundant interfaces is successfully designed synthesized. Benefiting from electron transfer behavior Mo , electrocatalysts C@CNF exhibit superior HER OER performance. Furthermore, when employed as anode cathode membrane electrode assembly devices, catalyst exhibits enhanced catalytic activity remarkable stability 100 hours at high current density 200 mA cm −2 towards overall splitting. experimental characterizations theoretical simulation reveal that modulation d‐band center C@CNF, achieved through asymmetric charge distribution resulting built‐in electric field induced by work function, enables optimization adsorption strength hydrogen/oxygen intermediates, thereby promoting kinetics This provides promising strategies designing highly active energy conversion fields.

Language: Английский

Citations

80

Manipulating Electron Redistribution in Ni2P for Enhanced Alkaline Seawater Electrolysis DOI Open Access
Xiaobin Liu,

Qingping Yu,

Xinyue Qu

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(1)

Published: Sept. 23, 2023

Abstract Developing bifunctional electrocatalyst for seawater splitting remains a persistent challenge. Herein, an approach is proposed through density functional theory (DFT) preanalysis to manipulate electron redistribution in Ni 2 P addressed by cation doping and vacancy engineering. The needle‐like Fe‐doped with (Fe‐Ni Pv) successfully synthesized on nickel foam, exhibiting superior hydrogen evolution reaction (HER) oxygen (OER) catalytic activity electrolysis alkaline condition. As result, Fe‐Ni Pv achieves the industrially required current densities of 1.0 3.0 A cm −2 at low voltages 1.68 1.73 V, respectively, 60 °C 6.0 m KOH circumstances. theoretical calculation experimental results collectively reveal reasons enhancement catalyst activity. Specifically, Fe vacancies can accelerate reconstruction OER active species optimize adsorption free energy (Δ G H* ) HER. In addition, sites are identified, where greatly improve electrical conductivity dominant centers, meanwhile atoms as centers study provides deep insight into exploration nickel‐based phosphide catalysts identification their real centers.

Language: Английский

Citations

73

Modulating Metal‐Nitrogen Coupling in Anti‐Perovskite Nitride via Cation Doping for Efficient Reduction of Nitrate to Ammonia DOI

Zhiheng Gong,

Xuepeng Xiang,

Wenye Zhong

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(38)

Published: Aug. 1, 2023

The complexes of metal center and nitrogen ligands are the most representative systems for catalyzing hydrogenation reactions in small molecule conversion. Developing heterogeneous catalysts with similar active metal-nitrogen functional centers, nevertheless, still remains challenging. In this work, we demonstrate that coupling anti-perovskite Co4 N can be effective modulated by Cu doping to form Co3 CuN, leading strongly promoted process during electrochemical reduction nitrate (NO3- RR) ammonia. combination advanced spectroscopic techniques density theory calculations reveal dopants strengthen Co-N bond upshifted d-band towards Fermi level, promoting adsorption NO3- *H facilitating transition from *NO2 /*NO H/*NOH. Consequently, CuN delivers noticeably better RR activity than pristine N, optimal Faradaic efficiency 97 % ammonia yield 455.3 mmol h-1 cm-2 at -0.3 V vs. RHE. This work provides an strategy developing high-performance catalyst synthesis.

Language: Английский

Citations

63

Inverse doping IrOx/Ti with weakened Ir-O interaction toward stable and efficient acidic oxygen evolution DOI Creative Commons
Yibo Wang,

Rongpeng Ma,

Zhaoping Shi

et al.

Chem, Journal Year: 2023, Volume and Issue: 9(10), P. 2931 - 2942

Published: July 5, 2023

Language: Английский

Citations

61

Work Function‐Guided Electrocatalyst Design DOI
Zhijie Chen, Tianyi Ma, Wei Wei

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(29)

Published: April 29, 2024

Abstract The development of high‐performance electrocatalysts for energy conversion reactions is crucial advancing global sustainability. design catalysts based on their electronic properties (e.g., work function) has gained significant attention recently. Although numerous reviews electrocatalysis have been provided, no such reports function‐guided electrocatalyst are available. Herein, a comprehensive summary the latest advancements in diverse electrochemical applications provided. This includes function‐based catalytic activity descriptors, and both monolithic heterostructural catalysts. measurement function first discussed descriptors various fully analyzed. Subsequently, function‐regulated material‐electrolyte interfacial electron transfer (IET) employed catalyst design, methods regulating optimizing performance discussed. In addition, key strategies tuning function‐governed material‐material IET examined. Finally, perspectives determination, put forward to guide future research. paves way rational efficient sustainable applications.

Language: Английский

Citations

59

Metal‐Organic Framework‐Based Electrocatalysts for Acidic Water Splitting DOI

Shenghao Zhou,

Lei Shi, Yanzhe Li

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(34)

Published: March 13, 2024

Abstract The proton exchange membrane water electrolysis system has long been considered a promising technique for the generation of hydrogen owing to its high electrolytic efficiency, reliability, and quick response renewable energy sources. At present, noble metals their oxides (e.g., Pt, IrO 2 , RuO ) are widely used as active electrocatalysts accelerating conversion efficiency process, especially in acidic media. Nevertheless, scarcity instability seriously impede large‐scale application practice. In past years, metal‐organic frameworks (MOFs) have proven be an ideal platform designing efficient cost‐effective electrodes due unique physicochemical properties. this review, fundamental catalytic mechanisms evolution reaction (HER) oxygen (OER) media discussed first. Then, design strategies advanced characterizations MOF‐based water‐splitting catalysts summarized. Finally, recent research advances HER OER electrolytes, along with current challenges future opportunities, provided.

Language: Английский

Citations

58

Activating lattice oxygen by a defect-engineered Fe2O3–CeO2 nano-heterojunction for efficient electrochemical water oxidation DOI Creative Commons

Qiuping Huang,

Guang‐Jie Xia, Bo Huang

et al.

Energy & Environmental Science, Journal Year: 2024, Volume and Issue: 17(14), P. 5260 - 5272

Published: Jan. 1, 2024

Self-supporting Fe 2 O 3 –CeO nano-heterojunction electrodes with rich oxygen vacancies present high catalytic performance for evolution reaction, where defect-engineering promotes the interfacial interaction and activates lattice oxygens.

Language: Английский

Citations

51