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

Lanke Luo,

Mingxuan Li,

Haohai Dong

et al.

ACS Catalysis, Journal Year: 2024, Volume and Issue: 15(1), P. 193 - 200

Published: Dec. 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.

Language: 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

et al.

Advanced Science, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 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.

Language: Английский

Citations

0
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

et al.

International Journal of Hydrogen Energy, Journal Year: 2025, Volume and Issue: 109, P. 287 - 294

Published: Feb. 11, 2025

Language: Английский

Citations

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

et al.

International Journal of Hydrogen Energy, Journal Year: 2025, Volume and Issue: 117, P. 110 - 120

Published: March 15, 2025

Language: Английский

Citations

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

et al.

ChemElectroChem, Journal Year: 2025, Volume and Issue: unknown

Published: March 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.

Language: Английский

Citations

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

et al.

Small, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 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.

Language: Английский

Citations

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

et al.

Inorganic Chemistry Communications, Journal Year: 2024, Volume and Issue: 172, P. 113720 - 113720

Published: Dec. 9, 2024

Language: Английский

Citations

1
Reconstructed Hydroxyl Coordination Field Enhances Mass Transfer for Efficient Electrocatalytic Water Oxidation DOI
Haomin Jiang,

Haohai Dong,

Yicheng Liu

et al.

Small, Journal Year: 2024, Volume and Issue: 21(6)

Published: Dec. 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.

Language: Английский

Citations

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

et al.

International Journal of Hydrogen Energy, Journal Year: 2024, Volume and Issue: 84, P. 372 - 382

Published: Aug. 20, 2024

Language: Английский

Citations

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

Lanke Luo,

Mingxuan Li,

Haohai Dong

et al.

ACS Catalysis, Journal Year: 2024, Volume and Issue: 15(1), P. 193 - 200

Published: Dec. 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.

Language: Английский

Citations

0