Precise modulation of electron spin states in metal-organic framework towards exceptional oxygen evolution reaction DOI Creative Commons
Minghua Huang,

Xianbiao Hou,

Tengjia Ni

et al.

Research Square (Research Square), Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 9, 2024

Abstract Spin configuration and coordination environment changes have emerged as promising strategies to boost the oxygen evolution reaction (OER) activity. However, achieving precise gradual regulation of both spin states elucidate structure-activity relationship remains a key priority is rarely reported. In this work, we successfully induce transition Fe sites from low state medium ultimately high by meticulously adjusting within NiFe-MOF, while Ni still keep state. Experimental theoretical calculations confirm polarization electrons migration Fe-t2g Fe-eg orbitals with reduced saturation, which optimizes orbital exchange interactions between ions facilitates adsorption intermediates. The NiFe-MOF-D3 unique NiO6-FeO4 geometric structure exhibits overpotential 328 mV@1 A cm-2 365 [email protected] in alkaline medium. Furthermore, assembled electrolyzer also presents remarkable activity (1.77 V@500 mA cm-2) lower cost ($ 0.94) than target U.S. Department Energy 2.00).

Language: Английский

Vacancy defect activation spin magnetic effect of Ni(OH)2 enhanced oxygen catalysis DOI
Tongyue Wang, Haomin Jiang, Cheng Zhang

et al.

International Journal of Hydrogen Energy, Journal Year: 2024, Volume and Issue: 72, P. 201 - 208

Published: May 29, 2024

Language: Английский

Citations

9
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

1
Superior Oxygen Evolution Electrocatalyst based on Ni‐Ellagic Acid Coordination Polymer DOI
Rui‐Lin Chai, Qian Zhao, Jie Li

et al.

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(27)

Published: May 11, 2024

Abstract The oxygen evolution reaction (OER) is central to energy conversion technologies, but the high cost and scarcity of commercial noble metal catalysts limit their widespread application. Natural products exhibit great potential in preparing high‐performance electrocatalysts due cost‐effectiveness sustainability. Here, a kind 1D polymers [M‐EA (M═Co, Cu, Ni)] for via complexation ellagic acid (EA) with ions are reported. It found that Ni‐EA displays low overpotential (190 mV at 10 mA cm −2 ) an ultralow Tafel slope (28 dec −1 ), production only 3.6 × % IrO 2 . Density functional theory investigations reveal electrocatalytic mechanism OER. A rechargeable Zn‐Air battery using Ni‐EA+Pt/C as air electrode shows lower charging better cycling stability than +Pt/C‐based battery. This work provides train development state‐of‐the‐art OER catalysts.

Language: Английский

Citations

8
Iron-Induced vacancy and electronic regulation of nickle phosphides for ampere-level alkaline water/seawater splitting DOI
Linbo Jiang,

Lintao Jiang,

Xu Luo

et al.

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 502, P. 157952 - 157952

Published: Nov. 28, 2024

Language: Английский

Citations

6
Catalysis under electric-/magnetic-/electromagnetic-field coupling DOI

Canyu Hu,

Yueyue Dong,

Qianqi Shi

et al.

Chemical Society Reviews, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 19, 2024

This review outlines recent advances in field-regulated catalysis and reveals the key role of dipole manipulation by electric/magnetic/electromagnetic fields.

Language: Английский

Citations

5
Tailoring Coordination Fields of Asymmetric MO5S1‐Type Metal–Organic Frameworks Catalysts for Accelerated Oxygen Evolution Reaction DOI

Tengjia Ni,

Xianbiao Hou,

Jian Zhou

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 27, 2024

Abstract Asymmetric coordination has emerged as a promising approach to enhance the oxygen evolution reaction (OER) activity, yet achieving controlled synthesis of asymmetric structures comprehensively understand structure‐activity relationship remains challenging. In this study, facile and effective symmetry‐breaking strategy is reported for tailoring MO 5 S 1 ‐type metal–organic frameworks (MOFs) catalyst, establishing correlation between sulfur (S)‐mediated electron rearrangement adsorption/desorption dynamics oxygen‐related intermediates in OER. Experimental theoretical calculations reveal that well‐designed structure can effectively lower d‐band center, optimizing adsorption behavior OH * significantly decreasing energy barrier rate‐determining step (OH → O ) with enhanced O–H bond cleavage process. The S‐NiFe‐MOF/CFP catalyst demonstrates remarkable OER performance an alkaline electrolyte environment. More importantly, self‐assembled anion exchange membrane water electrolysis cell showcases low voltage 1.84 V deliver current density A cm −2 , maintaining long‐term stability over 100 h. This study unveils precise employing S, highlighting critical role manipulating redistribution through promote catalytic activity develop advanced MOF‐based catalysts.

Language: Английский

Citations

4
Single-atomic iron synergistic atom-cluster induce remote enhancement toward oxygen reduction reaction DOI

Yayin Li,

Haomin Jiang, Liu Lin

et al.

Journal of Energy Chemistry, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 1, 2024

Language: Английский

Citations

4
Tuning the Spin State of Co Accelerates Hydrogen Evolution Reaction of Pt Nanoparticles DOI Creative Commons
Qian Zheng, Wei An, Jianxin Pan

et al.

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

Published: Jan. 16, 2025

ABSTRACT The quest for dynamic and cost‐effective electrocatalysts to substitute carbon‐supported platinum (Pt) in alkaline hydrogen evolution reaction (HER) remains a pressing challenge. incorporation of transition metal atoms through electron donation spin regulation dominates the HER performance Pt nanoparticles. Herein, we demonstrate that Co‐N coordination was utilized regulate stabilize chemical microenvironment nanoparticles fabricate hybrid (Pt/CoNC). resultant Pt/CoNC delivers ultralow overpotentials 15.2 171.2 mV at current densities 10 100 mA cm −2 , surpassing commercial Pt/C. poisoning tests, where η values depict negative shifts 161 13 by potassium thiocyanide (KSCN) ethylenediaminetetraacetic acid disodium (EDTA), suggest combined impact on HER, with playing decisive role. magnetic characterization density diagrams reveal induces higher state Co 2+ creating wider spin‐related channel Pt. Moreover, effectively modifies electronic structure Pt, thereby reducing energy barriers H 2 O dissociation (from 0.41 −0.22 eV) generation −0.35 0.03 eV). This finding provides insights advanced regulating modulating interfacial transfer.

Language: Английский

Citations

0
Precisely regulating the electronic configuration of Fe-N4 units for practical oxygen reduction reactions DOI
Hui Zhang, Jingjing Jiang, Baojie Li

et al.

Chemical Engineering Journal, Journal Year: 2025, Volume and Issue: unknown, P. 159888 - 159888

Published: Jan. 1, 2025

Language: Английский

Citations

0
Modulation of Co spin state at Co3O4 crystalline-amorphous interfaces for CO oxidation and N2O decomposition DOI Creative Commons
Yunpeng Long, Xiao‐Wei Zhu, Chuan Gao

et al.

Nature Communications, Journal Year: 2025, Volume and Issue: 16(1)

Published: Jan. 26, 2025

Modulation of electronic spin states in cobalt-based catalysts is an effective strategy for molecule activations. Crystalline-amorphous interfaces often exhibit unique catalytic properties due to disruptions long-range order and alterations structure. However, the mechanisms activation at remain elusive. Herein, we present a Co3O4 spinel-based catalyst featuring crystalline-amorphous interfaces. Characterization analyses confirm that tetrahedral Co2+ selectively etched from bulk spinel, forming amorphous CoO islands on surface. The resultant symmetry breaking coordination field induces reconstruction Co3+ 3 d orbitals, leading high-spin states. In CO oxidation, interface serves as novel active sites with lower energy barrier, facilitated by lattice oxygen activation. N2O decomposition, promotes reassociation dissociated through quantum exchange interactions. This work provides straightforward approach modulating state elucidates their role properties, but molecular these study presents

Language: Английский

Citations

0