CHINESE JOURNAL OF CATALYSIS
·
2025
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IF 17.7
Jiangyu Tang,Xiao Wang,Yunfa Wang,Min Shi,Peng Huo,Jianxiang Wu,Qiaoxia Li,Qunjie Xu
The oxygen evolution reaction (OER) serves as a fundamental half–reaction in the electrolysis of water for hydrogen production, which is restricted by the sluggish OER reaction kinetics and unable to be practically applied. The traditional lattice oxygen oxidation mechanism (LOM) offers an advantageous route by circumventing the formation of M-OOH* in the adsorption evolution mechanism (AEM), thus enhancing the reaction kinetics of the OER but resulting in possible structural destabilization due to the decreased M–O bond order. Fortunately, the asymmetry of tetrahedral and octahedral sites in transition metal spinel oxides permits the existence of non-bonding oxygen, which could be activated by rational band structure design for direct O-O coupling, where the M–O bond maintains its initial bond order. Here, non-bonding oxygen was introduced into NiFe 2 O 4 via annealing in an oxygen-deficient atmosphere. Then, in-situ grown sulfate species on octahedral nickel sites significantly improved the reactivity of the non-bonding oxygen electrons, thereby facilitating the transformation of the redox center from metal to oxygen. LOM based on non-bonding oxygen (LOM NB ) was successfully activated within NiFe 2 O 4 , exhibiting a low overpotential of 206 mV to achieve a current density of 10 mA cm –2 and excellent durability of stable operation for over 150 h. Additionally, catalysts featuring varying band structures were synthesized for comparative analysis, and it was found that the reversible redox processes of non-bonding oxygen and the accumulation of non-bonding oxygen species containing 2 p holes are critical prerequisites for triggering and sustaining the LOM NB pathway in transition metal spinel oxides. These findings may provide valuable insights for the future development of spinel-oxide-based LOM catalysts.
研究领域:
材料科学
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电化学
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Nano
·
2024
·
IF 15.8
Qingming Deng,Hui Li,Ke Pei,Lok Wing Wong,Xiaodong Zheng,Chi Shing Tsang,Honglin Chen,Wenqian Shen,Thuc Hue Ly,Jiong Zhao,Qiang Fu
High-efficiency catalysts with refined electronic structures are highly desirable for promoting the kinetics of the oxygen evolution reaction (OER) and enhancing catalyst durability. This study comprehensively explores strategies involving metal doping and oxygen vacancies for enhancing the acidic OER catalytic activity of Co3O4. Through extensive screening of 3d and 4d transition metals using density functional theory (DFT) simulations, we demonstrate that the incorporation of metal dopants and oxygen vacancies into Co3O4 potentially triggers a transition from the adsorbate evolution mechanism (AEM) to the lattice oxygen oxidation mechanism (LOM) in the oxygen evolution reaction (OER). While the formation of the O–O bond in the intermediate *OOH poses challenges, a significantly reduced overpotential facilitates efficient conversion of O to O2 through the LOM in *OH and lattice oxygen. Additionally, we find that Mn doping can significantly improve the stability of the catalyst. Building upon the rationale above, we employed a dual doping strategy in subsequent experiments to enhance both the activity and stability. Our final design involved the codoping of Mn and Ru in Co3O4, along with an appropriate amount of oxygen vacancies. This catalyst demonstrates a low overpotential (η10 = 230 mV) compared to pure Co3O4 and maintains stable operation for over 120 h, representing a 12-fold increase. By exploring and harnessing the LOM, more efficient, stable, and cost-effective OER catalysts can be designed, providing crucial support for technologies such as water electrolysis in clean energy.
研究领域:
材料科学
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催化化学
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清洁能源技术
✓ 已验证
DOI
PubMed
高影响因子
Science Advances
·
2022
·Vol. 8
·期 30
·
IF 14.957
Min Lu,Yao Zheng,Yang Hu,Bolong Huang,Deguang Ji,Mingzi Sun,Jianyi Li,Yong Peng,Rui Si,Pinxian Xi,Chun-Hua Yan
The regulation of mechanism on the electrocatalysis process with multiple reaction pathways is more efficient and essential than conventional material engineering for the enhancement of catalyst performance. Here, by using oxygen evolution reaction (OER) as a model, which has an adsorbate evolution mechanism (AEM) and a lattice oxygen oxidation mechanism (LOM), we demonstrate a general strategy for steering the two mechanisms on various LaxSr1−xCoO3−δ. By delicately controlling the oxygen defect contents, the dominant OER mechanism on LaxSr1−xCoO3−δ can be arbitrarily transformed between AEM-LOM-AEM accompanied by a volcano-type activity variation trend. Experimental and computational evidence explicitly reveal that the phenomenon is due to the fact that the increased oxygen defects alter the lattice oxygen activity with a volcano-type trend and preserve the Co0 state for preferably OER. Therefore, we achieve the co-optimization between the activity and stability of catalysts by altering the mechanism rather than a specific design of catalysts.
研究领域:
电化学
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催化科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Tixuan Xia,Chunbo Liu,Yang Lu,Wei Jiang,Hongji Li,Yunchao Ma,Yuanyuan Wu,Guangbo Che
Oxygen evolution reaction is one of the core half-reactions in proton-exchange membrane (PEM) water electrolysis, but its slow reaction kinetics has been limiting the overall energy conversion efficiency (e.g., water splitting). It is urgent to develop efficient catalysts for OER in acidic media. At present, Ru-based catalysts have high activity, but their poor stability makes them difficult to be used in acidic oxygen evolution reactions. The involvement of lattice oxygen mechanism (LOM) in the reaction is one of the main causes of instability in Ru-based catalysts. Herein, we synthesized SrRu 0.5 Ir 0.5 O 3 double perovskite by doping Ir into SrRuO 3 . The double perovskite displays an extraordinary OER performance with a low overpotential of 185 mV at 10 mA cm −2 current density and maintains its catalytic stability for over 50 h in 0.5 M H 2 SO 4 . X-ray photoelectron spectroscopy results show that the electronic synergistic effect between Ir and Ru enables the double perovskite materials with high activity. Meanwhile, the double perovskite catalyst inhibits the occurrence of the lattice oxygen mechanism during the OER, which greatly improve the catalytic stability of Ru-based perovskite materials.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2025
·
IF 4.1
Zihang Feng,Zhe Zhang,Xiaoxuan Zhang,Jinsheng Li,Xuefei Lei,Xuanwen Liu
The oxygen evolution reaction (OER)is crucial for the development of energy storage technologies such as water splitting for hydrogen production and metal-air batteries; therefore, developing efficient electrocatalysts is key to advancing OER. NiFe₂O₄, as a typical spinel-structured transition metal oxide, features nickel ions Ni 2+ preferentially occupying tetrahedral sites and iron ions Fe 3+ occupying octahedral sites within its crystal lattice. This unique dual-metal site distribution significantly optimizes the adsorption energy of oxygen intermediates through Ni Fe electronic synergy, overcoming the inherent activity limitations of single-metal oxides. Simultaneously, its high electrical conductivity and robust stability in alkaline environments make it an ideal alternative to precious metal catalysts. However, its intrinsic activity remains constrained by the sluggish kinetics of the conventional adsorbate evolution mechanism (AEM) and insufficient exposure of surface active sites. To address this, this study focuses on a breakthrough modification of nickel ferrite NiFe₂O₄: employing a phosphorus doping strategy, the reaction mechanism is successfully transformed from the AEM to the lattice oxygen oxidation mechanism (LOM) during the heating process, with optimization of heating time and temperature parameters. The optimized phosphorus-doped nickel ferrite NFO − P achieves a low overpotential of 229 mV and a Tafel slope of 75.1 mV dec −1 at a current density of 10 mA cm −2 —its performance significantly surpasses that of pristine NiFe₂O₄ and approaches the level of precious metal IrO₂. This work concurrently reveals that phosphorus doping overcomes the activity limitations of the traditional AEM pathway by weakening metal‑oxygen bonds and activating lattice oxygen, thereby providing a reference for “AEM → LOM” mechanism regulation in transition metal oxide catalysts.
研究领域:
电化学
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材料科学
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储能
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催化
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纳米技术
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Weilin Shen,Xiao Chen,Huibin Liu,Wenhao Yang,Wenjun Zhu,Mingyu Xie,Mengfan Hao,Tamás Ollár,Pei Yuan,Changhai Liang
The rational design of high-efficiency electrocatalysts with tailored geometric configurations and optimized electronic properties has emerged as a critical strategy for simultaneously accelerating oxygen evolution reaction (OER) kinetics and enhancing catalyst durability in electrochemical water splitting systems. In this work, the application of high-entropy design to spinel oxides effectively integrates the unique spinel structure with refined electronic characteristics inherent in high-entropy metal oxides, endowing the spinel-type high-entropy oxide (Fe 0.2 Co 0.2 Ni 0.2 Mn 0.2 Zn 0.2 ) 3 O 4 -700 with excellent OER performance and stability. The highly dispersed (Fe 0.2 Co 0.2 Ni 0.2 Mn 0.2 Zn 0.2 ) 3 O 4 -700/CC electrode catalyst exhibits remarkable OER performance, with a low overpotential of 313 mV at 10 mA cm −2 and a Tafel slope of 59.7 mV dec −1 , alongside outstanding stability (only 9 mV degradation after 150 h of operation). This OER performance is significantly superior to both monometallic and bimetallic oxides. Structural analyses reveal dynamic surface reconstruction during the OER, resulting in the formation of an amorphous high-entropy oxyhydroxide (FeCoNiMnZnOOH) shell via the co-hydroxylation of the five metallic components. This surface intermediate promotes the formation of O 2 via the lattice oxygen oxidation mechanism. This unique combination of surface adaptability and bulk stability enables both high activity and durability. This research highlights high-entropy spinels as promising OER catalysts, providing both fundamental insights and practical potential for sustainable energy applications.
研究领域:
材料科学
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电化学
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催化
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能量转换
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纳米技术
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2024
·
IF 15.7
Jia Liu,Shibin Wang,Jinfu Cai,Lizhen Wu,Yun Liu,Jiahui He,Zaixiang Xu,Xiaoge Peng,Xing Zhong,Liang An,Jianguo Wang
Electrochemical ozone production (EOP) is an intrinsically safe technology compared to Corona discharge methods for ozone generation. However, EOP technology exhibits higher electrical utility demand. Herein, a square-shaped lead oxide (PbO x -CTAB-120) electrocatalyst with outstanding EOP activity has been successfully prepared by a simple method. Then the PbO x -CTAB-120 was assembled into a newly visualized EOP electrolyzer (with parallel flow field) at 1.0 A cm −2 in ultrapure water. The gaseous ozone yield reached 588 mg h −1 g −1 catalyst , corresponding to a specific energy consumption (P EOP ) of 56 Wh g −1 gaseous ozone . In-situ 18 O isotope-labelled differential electrochemical mass spectrometry reveals that PbO x -CTAB-120 undergoes phase shuttling to β-PbO 2 via the lattice oxygen oxidation mechanism pathway. Furthermore, density functional theory calculations for multiple reaction pathways on the Pb 3 O 4 (110) surface also demonstrated the participance of lattice oxygen in the EOP process, with the results show that the oxygen vacancy generated from lattice oxygen migration could effectively stabilize the OOH* and O 2 * reaction intermediate in contrast to the adsorbate evolution mechanism. Therefore, the presence of highly stabilized surfaces Pb 3 O 4 (110) on PbO x -CTAB-120 before phase shuttling and the stabilization of β-PbO 2 (101) and β-PbO 2 (110) crystalline surfaces after phase shuttling allowed PbO x -CTAB-120 to maintain its excellent EOP activity and stability. Moreover, based on computational fluid dynamics simulations and experimental observations, the parallel flow field design facilitated efficient mass transfer of the gaseous product (O 2 +O 3 ) and effective thermal dissipation of the system. In addition, the high activity electrocatalyst coupled with the optimized EOP electrolyzer enabled efficient in-situ degradation of organic species.
研究领域:
电化学
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催化
·
环境科学
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材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）