Manipulating Metal Cations Microenvironment for Highly Selective Electrochemical Water Oxidation to Hydrogen Peroxide DOI

Lanke Luo,

Mingxuan Li,

Haohai Dong

и другие.

ACS Catalysis, Год журнала: 2024, Номер 15(1), С. 193 - 200

Опубликована: Дек. 16, 2024

Electrochemical two-electron water oxidation (2e– WOR) represents a promising approach for the renewable and on-site production of H2O2, potentially replacing anthraquinone process. Nevertheless, it faces intense competition from conventional four-electron oxygen evolution reaction (OER), resulting in low selectivity, high overpotential, yield. Herein, taking carbon-based structures with 2e– WOR selectivity as model catalysts, by manipulating electrolyte, increased maximum Faraday efficiency H2O2 to 71 ± 3%, an rate 11.7 μmol cm–2 min–1. The activity was found be most sensitive alkali metal cations following order: Cs+ > K+ Na+ Li+. In situ spectroscopy characterization confirmed that larger facilitate generation peroxide species; this is because, on one hand, can regulate electronic catalyst sites improve adsorption intermediates; other cation-hydrogen interaction regulates stable coordination cation, realizes reforming hydrogen bond network, prevents its further into O2. With help flow electro-synthetic cell, we successfully achieve rapid degradation organic pollutants preparation solid (sodium peroxycarbonate). This work not only enriches understanding cationic mechanisms but also provides implications rational optimization strategies electrode/electrolyte interface.

Язык: Английский

Spin Magnetic Effect Activate Dual Site Intramolecular O─O Bridging for Nickel‐Iron Hydroxide Enhanced Oxygen Evolution Catalysis DOI Creative Commons

Haohai Dong,

Lanke Luo,

Shaobing Zhou

и другие.

Advanced Science, Год журнала: 2025, Номер unknown

Опубликована: Янв. 21, 2025

Abstract The oxygen evolution reaction (OER) involves the recombination of diamagnetic hydroxyl (OH) or water (H 2 O) into paramagnetic triplet state (O ). spin conservation intermediates plays a crucial role in OER, however, research on dynamics during catalytic process remains its early stages. Herein, β ‐Ni(OH) and Fe‐doped (Ni 5 Fe 1 ) are utilized as model catalysts to understand mechanism magnetic effects at iron (III) sites OER. Combined with characterization, it is founded that introduction transforms antiferromagnetic Ni(OH) ferromagnetic material. Testing response catalyst under an external field, OER activity Ni significantly enhanced comparison . This improvement likely due sites, which promote enhance kinetics, thereby increasing efficiency. Combining experimental theoretical discovered accelerate formation heterogeneous dual‐site O─O bridging, represented ─Ni─O─O─Fe─, effectively enhancing kinetics reaction. study provides perspective structure‐function relationship iron‐based has significant implications for design new catalysts.

Язык: Английский

Процитировано

1
Oxygen vacancy-rich nickel-iron layered double hydroxide nanosheets wrapped nickel-cobalt hybrid sulfides as efficient electrocatalysts for oxygen evolution reaction DOI

Yuqian Gao,

Peng Cui,

Tao Gu

и другие.

International Journal of Hydrogen Energy, Год журнала: 2025, Номер 109, С. 287 - 294

Опубликована: Фев. 11, 2025

Язык: Английский

Процитировано

0
Tailoring the bifunctional electrocatalytic activity of nickel-cobalt sulfides derived from ZIF-67 by cerium doping to enhance the overall water splitting performance DOI
Lei Tian,

Jin Liang,

Y. Zhang

и другие.

International Journal of Hydrogen Energy, Год журнала: 2025, Номер 117, С. 110 - 120

Опубликована: Март 15, 2025

Язык: Английский

Процитировано

0
Modulating Electronic Spin State of Perovskite Fluoride by Ni─F─Mn Bond Activating the Dynamic Site of Oxygen Reduction Reaction DOI Open Access
Shuang Yang,

Jiaqin Chen,

Rong Li

и другие.

Small, Год журнала: 2025, Номер unknown

Опубликована: Янв. 23, 2025

Abstract Establishing the relationship between catalytic performance and material structure is crucial for developing design principles highly active catalysts. Herein, a type of perovskite fluoride, NH 4 MnF 3 , which owns strong‐field coordination including fluorine ammonia, in situ grown on carbon nanotubes (CNTs) used as model to study improve intrinsic activity through heteroatom doping strategies. This approach optimizes spin‐dependent orbital interactions alter charge transfer catalyst reactants. As result, oxygen reduction reaction (ORR) CNTs significantly enhanced by partial substitution Mn sites with Ni, such half‐wave potential (E 1/2 ) 0.86 V limiting current density 5.26 mA cm −2 are comparable those commercial Pt/C Experimental theoretical calculations reveal that introduction Ni promotes lattice distortion, adjusts electronic states centers, facilitates transition from low‐spin intermediate‐spin states, shifts d ‐band center closer Fermi level. establishes novel designing high‐performance perovskite‐based fluoride electrocatalysts modulating spin states.

Язык: Английский

Процитировано

0
The Design of Spin Catalysts: Breakthroughs toward Efficient Energy Conversion DOI Creative Commons
Yantao Yang, Yufeng Li, Baipeng Yin

и другие.

ChemElectroChem, Год журнала: 2025, Номер unknown

Опубликована: Март 30, 2025

In energy conversion technologies, the electron spin effect in catalysts plays a crucial role overcoming spin‐forbidden reactions, offering novel approach to overcome performance bottlenecks of catalysts. Recently, with breakthroughs magnetic field–enhanced catalysis and theoretical predictions, significant progress has been made design development this concept, several attractive inspiring catalyst strategies reported recently, particularly precise modulation states/spin interactions at catalytic sites through coordination modulation, spin‐pinning effect, chirality induction, radical adsorption, are outlined. The concept then explores advantages these enhancing activity/selectivity, investigating selectivity reaction pathways, expanding systems. Finally, proposes future directions for technologies.

Язык: Английский

Процитировано

0
Magnetically Tuned Spintronic Interfaces in Electrocatalysis: Advanced Mechanistic Understanding, Reactivity Kinetics and Challenges DOI
Saira Ajmal, Junfeng Huang, Anuj Kumar

и другие.

Nano Energy, Год журнала: 2025, Номер unknown, С. 111134 - 111134

Опубликована: Май 1, 2025

Язык: Английский

Процитировано

0
Structural, optical, chromaticity, and magnetic properties of uncapped and reduced graphene oxide (rGO) capped-β-Ni(OH)2 nanostructures for spintronic devices, and LED applications DOI

J. Gajendiran,

J. Ramana Ramya,

S. Gnanam

и другие.

Inorganic Chemistry Communications, Год журнала: 2024, Номер 172, С. 113720 - 113720

Опубликована: Дек. 9, 2024

Язык: Английский

Процитировано

2
Reconstructed Hydroxyl Coordination Field Enhances Mass Transfer for Efficient Electrocatalytic Water Oxidation DOI
Haomin Jiang,

Haohai Dong,

Yicheng Liu

и другие.

Small, Год журнала: 2024, Номер 21(6)

Опубликована: Дек. 29, 2024

Abstract Mass transfer factor plays an indispensable role in high current density to accelerate the oxygen evolution reaction (OER) process, yet research on modulating reactant mass transport remains limited. Herein, by leveraging dual acid‐base properties of aluminum sites, both activation electronic activity layer for layered double hydroxides (LDH) and construction interlayer hydroxide coordination field (IHCF) have been achieved through situ electrochemical reconstruction. It not only facilitates charge surface catalytic transformation intermediates but, most notably, presence IHCF significantly enhances reactants. As a result, overpotential LDHs with is 164 mV, better than reported Ni‐based catalysts. Deuterium kinetic isotope effect experiments pH‐dependence measurements demonstrate that effectively substrate capability structural stability, thereby accelerating proton‐coupled electron process. To further validate characteristics, stability tests alkaline flow electrolyzer show catalysts maintain over 1000 h at density. This work suggests can be utilized design synthesis efficient water oxidation practical application.

Язык: Английский

Процитировано

1
The 2D porous NiSe/g-C3N4 nanosheets towards enhanced photocatalytic H2 evolution and degradation via synergism of co-catalyst and surface protonation DOI

Shaoyu Song,

Yujia Huang,

Jiachang Lian

и другие.

International Journal of Hydrogen Energy, Год журнала: 2024, Номер 84, С. 372 - 382

Опубликована: Авг. 20, 2024

Язык: Английский

Процитировано

0
Manipulating Metal Cations Microenvironment for Highly Selective Electrochemical Water Oxidation to Hydrogen Peroxide DOI

Lanke Luo,

Mingxuan Li,

Haohai Dong

и другие.

ACS Catalysis, Год журнала: 2024, Номер 15(1), С. 193 - 200

Опубликована: Дек. 16, 2024

Electrochemical two-electron water oxidation (2e– WOR) represents a promising approach for the renewable and on-site production of H2O2, potentially replacing anthraquinone process. Nevertheless, it faces intense competition from conventional four-electron oxygen evolution reaction (OER), resulting in low selectivity, high overpotential, yield. Herein, taking carbon-based structures with 2e– WOR selectivity as model catalysts, by manipulating electrolyte, increased maximum Faraday efficiency H2O2 to 71 ± 3%, an rate 11.7 μmol cm–2 min–1. The activity was found be most sensitive alkali metal cations following order: Cs+ > K+ Na+ Li+. In situ spectroscopy characterization confirmed that larger facilitate generation peroxide species; this is because, on one hand, can regulate electronic catalyst sites improve adsorption intermediates; other cation-hydrogen interaction regulates stable coordination cation, realizes reforming hydrogen bond network, prevents its further into O2. With help flow electro-synthetic cell, we successfully achieve rapid degradation organic pollutants preparation solid (sodium peroxycarbonate). This work not only enriches understanding cationic mechanisms but also provides implications rational optimization strategies electrode/electrolyte interface.

Язык: Английский

Процитировано

0