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

Efficient H2O2 Synthesis through a Two‐Electron Oxygen Reduction Reaction by Electrocatalysts DOI

Huatian Chen,

Runxuan Chen,

Sha Liu

et al.

ChemPlusChem, Journal Year: 2024, Volume and Issue: 89(11)

Published: July 16, 2024

Abstract The two‐electron oxygen reduction reaction (2e‐ORR) for the sustainable synthesis of hydrogen peroxide (H 2 O ) has demonstrated considerable potential local production this environmentally friendly chemical oxidant on small, medium, and large scales. This method offers a promising alternative to energy‐intensive anthraquinone approach, placing primary emphasis development efficient electrocatalysts. Improving efficiency electrocatalysts uncovering their catalytic mechanisms are essential steps in achieving high 2e‐ORR activity, selectivity, stability. comprehensive review summarizes recent advancements in‐situ H production, providing detailed overview field. In particular, delves into design, fabrication, investigation active sites contributing selectivity. Additionally, it highlights range including pure metals alloys, transition metal compounds, single‐atom catalysts, carbon‐based catalysts pathway. Finally, addresses significant challenges opportunities electrosynthesis, as well future research directions.

Language: Английский

Citations

9

Strategies to maximize the oxygen evolution reaction in layered double hydroxides by electronic defect engineering DOI Creative Commons

Heyu Zhou,

Jinjin Ban, Yonglong Shen

et al.

eScience, Journal Year: 2025, Volume and Issue: unknown, P. 100380 - 100380

Published: Feb. 1, 2025

Language: Английский

Citations

1

Dynamic evolution processes in electrocatalysis: structure evolution, characterization and regulation DOI
Chao Xie, Wei Chen, Yanyong Wang

et al.

Chemical Society Reviews, Journal Year: 2024, Volume and Issue: 53(22), P. 10852 - 10877

Published: Jan. 1, 2024

Dynamic evolution processes in electrocatalysis, including structure of electrocatalysts, characterization methods and regulation strategies for dynamic electrocatalysis.

Language: Английский

Citations

5

Quantum fundaments of catalysis: true electronic potential energy DOI
José Gracia, Chiara Biz, Mauro Fianchini

et al.

Physical Chemistry Chemical Physics, Journal Year: 2024, Volume and Issue: 26(34), P. 22620 - 22639

Published: Jan. 1, 2024

Catalysis is a quantum phenomenon enthalpically driven by electronic correlations with many-particle effects in all of its branches, including electro-photo-catalysis and electron transfer. This means that only probability amplitudes provide complete relationship between the state catalysis observations. Thus, any atomic system material), competing space-time interactions coexist to define (related) properties such as stability, (super)conductivity, magnetism (spin-orbital ordering), chemisorption catalysis. Catalysts, reactants, chemisorbed transition states have possibility optimizing improve reaction kinetics. Active sites closed-shell orbital configurations share maximum number spin-paired electrons, mainly coulombic attractions covalency defining weakly correlated (WCCS) structures. However, compositions open-shell configurations, at least, spin exchange (QSEIopenshells) arise, stabilising unpaired electrons less covalent bonds differentiating non-weakly (or strongly) (NWCOS) systems. In NWCOS catalysts, ground can diverse rival spin-orbital orderings well ferro-, ferri- multiple antiferro-magnetic textures, which deeply their activities. Particularly inter-atomic ferromagnetic (FM) bonds, increase relevance non-classical potentials significantly optimize energies, (TSs), activation energies (overpotential) spin-dependent transfer (conductivity), overall implying need for explaining thermodynamic kinetic origin from true energy. To do so, we use connection Born-Oppenheimer approximation Virial theorem treatment potential energies. exact fundamental decompose TSs appear. The increasing stabilization TSs, due on NWCO opens simultaneously reducing enthalpies barriers mechanisms, implies anticipation explanation positive deviations Brønsted-Evans-Polanyi principle.

Language: Английский

Citations

4

Co-based Spinel and Perovskite Oxides in Catalytic Combustion of Volatile Organic Compounds: Recent Advances and Future Prospects DOI

Zijuan You,

Tongyu Liu, Meiqin Chen

et al.

Journal of environmental chemical engineering, Journal Year: 2025, Volume and Issue: 13(1), P. 115359 - 115359

Published: Jan. 7, 2025

Language: Английский

Citations

0

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

Asymmetric optical waveguide in one‐dimensional organic microplate DOI Creative Commons

Ziyi Yuan,

Xiu‐Fen Cheng,

Zejian Li

et al.

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

Published: Feb. 4, 2025

Abstract Chiral organic materials have garnered significant interest in nanophononics due to their ability manipulate polarized light and encode optical information. Herein, chiral one‐dimensional (1D) microplates based on benzocyclazine form homochiral crystals that exhibit excellent waveguiding properties. These exhibited highly asymmetric propagation depends the handedness of circularly (CPL). demonstrated selective transmission, with R ‐microplate favouring left‐handed CPL S right‐handed CPL, showcasing distinct loss coefficients for each enantiomer. Multichannel was observed, where intensity varied excitation position. results highlight potential 1D advanced nanophotonic devices, offering chiral‐dependent control over transmission future applications information processing.

Language: Английский

Citations

0

Advances in Spinel-Type Electrocatalysts: Leveraging Ligand Field Theory to Elucidate Structure-Property Relationships DOI Creative Commons
Xin Li, Zongkui Kou,

Jiayan Dai

et al.

Journal of Materiomics, Journal Year: 2025, Volume and Issue: unknown, P. 101031 - 101031

Published: Feb. 1, 2025

Language: Английский

Citations

0

Asymmetry Spin‐Orbit of Single Iron Active Site Enhance Oxygen Reduction Reaction DOI

Yayin Li,

Haomin Jiang,

Yu He

et al.

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

Published: Feb. 25, 2025

Abstract Asymmetric electron distribution of single‐atom catalysts (SAC) is an important means regulating intrinsic catalytic activity. However, limited by synthetic preparation methods, understanding the mechanism asymmetrically coordinated catalysis restricted. In this study, leveraging micropore confinement effect, nitrogen and phosphorus‐doped microporous carbon used as a substrate to successfully anchor singly dispersed Fe atoms, constructing site with N P atoms (Fe‐SAs/NPC). The existence Fe‐N 3 1 structure breaks symmetry 4 in Fe‐SAs/NC, which would optimize adsorption strength intermediates. resulting Fe‐SAs/NPC exhibits excellent ORR activity half‐wave potential 0.91 V (0.1 m KOH), 40 mV higher than that Fe‐SAs/NC (0.87 V). Combined theoretical calculations, in‐depth asymmetric electronic configuration from perspective spin orbitals can enhance near Fermi level strengthen oxygen‐containing This work provides new perspectives ideas for spin‐electronic behavior processes. Furthermore, Zn‐air battery constructed using high power density 187.7 mW cm −2 specific capacity 819.6 mAh g Zn −1 at 10 mA .

Language: Английский

Citations

0

External field-assisted catalysis DOI Creative Commons
Linbo Jiang,

Lintao Jiang,

Xu Luo

et al.

eScience, Journal Year: 2025, Volume and Issue: unknown, P. 100398 - 100398

Published: March 1, 2025

Language: Английский

Citations

0