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Advanced Energy Materials · 2024 · IF 24.4

Multihybridization for Enhancing Fe-Ni Bimetal Electrocatalyst in Water Oxidation

Hongyan Zhang,Hao Zhou,Hua Wang,Yikai Wang,Xuehan Yang,Dan Wu,Pan Yuan,Maoshuai He,Wenxian Wei,Tao Yang

Water electrolysis holds the promise of transforming electric-power into hydrogen energy through a carbon free process and its widespread application highly depends on anodic oxygen evolution reaction (OER) efficiency. Transition metal-based OER catalysts meet the requirements of long-term development for cost effectiveness, and their performance can be improved by a variety of band electronic structure modulating methods. Herein, a multihybridization strategy is proposed, i.e., p-d, s-sp , and d-d hybridization are emphasized together, which guides the design of an effective vanadium (V), boron (B)-FeNiP catalyst. Density functional theory analysis reveals the existence of multihybridization and the difference between Fe and Ni in terms of hybridization strength, band configuration, and interfacial charge transfer. Specially, Fe and Ni sites are simultaneously optimized to their highest performance upon the dual B, V incorporation. As a result, the VB-FeNiP catalyst displays outstanding OER performance, regarding a Tafel slope of 57.64 mV dec −1 , an overpotential of 175 mV at 100 mA cm −2 , and exceptional stability. Here the synergistic effect of multihybridization in the design of transition metal-based catalysts is highlighted and the work in pursuit of effective way based on regulating band configuration to developing high performance OER catalysts would be evoked.

研究领域: 材料科学 · 电化学
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CARBON · 2020 · IF 8.821

ORR and OER of Co–N codoped carbon-based electrocatalysts enhanced by boundary layer oxygen molecules transfer

Jintao Zhang,Tong Zhang,Jing Ma,Zhi Wang,Junhao Liu,Xuzhong Gong

Two-step carbonization method was reported to synthesize Co–N doped coal tar pitch (CTP) carbon-based electrocatalysts with hierarchical pore structure , high local order degree and efficient Co-N x active structure simultaneously. The synergistic effect of the carbon substrate with highly ordered structure and the Co-N x active sites realized the “Point discharge effect”. The π-π interactions from the CTP aromatic ring sheets and Co-N x promoted the adsorption and dissociation of oxygen molecules, respectively. The increased diffusion coefficient ( D 0 ) indicated the mass transfer of oxygen molecules in the boundary layer was enhanced during the ORR process. Thanks to excellent structural characteristics, ACTP 5 @Co,N-800 exhibited better ORR performance than commercial Pt/C catalyst under alkaline conditions, and the OER activity was improved simultaneously. This work demonstrated a simple and practical strategy for the development of advanced carbon-based electrocatalysts, and also provided novel insights from kinetics perspectives for improving electrocatalytic efficiency.

CAS / MDL: 10026-22-9
研究领域: 材料科学 · 电化学
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Materials · 2024 ·Vol. 17 ·期 19 ·4876 · IF 3.1

Improved HER/OER Performance of NiS2/MoS2 Composite Modified by CeO2 and LDH

Hao Li,Feng Chen,Xinyang Wu,Dandan Wang,Yongpeng Ren,Yaru Li

In recent years, there has been significant interest in transition-metal sulfides (TMSs) due to their economic affordability and excellent catalytic activity. Nevertheless, it is difficult for TMSs to achieve satisfactory performance due to problems such as low conductivity, limited catalytic activity, and inadequate stability. Therefore, a catalyst with a heterostructure constituted of a nickel–iron-layered double hydroxide, nickel sulfide, molybdenum disulfide, and cerium dioxide was designed. At the current density of 10 mA cm−2in an alkaline solution, the catalyst exhibits a HER overpotential of 116 mV. In addition, an overpotential of 235 mV@150 mA cm−2was displayed for OER. The catalyst showed a good retention rate (94.7% for HER, 98.6% for OER) after 160 h stability tests. The excellent electrochemical performance is attributed to the following points: 1. The self-supporting three-dimensional hierarchical structure provides abundant sites, fast ion diffusion channels, and electron transfer paths, and ensures structural stability. 2. The strong interfacial electron interaction between Ni3S2/MoS2heterojunction and NiFe-LDH improves the OER reaction kinetics. 3. The Ce3+and oxygen vacancies in CeO2promote the dissociation of H2O and promote the HER reaction kinetics. This approach paves the way for developing highly efficient electrocatalysts for various electrochemical applications.

研究领域: 材料科学 · 电化学
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2025 · IF 8.3

Na-modified La(CrMnFeCoNi)1/5O3 high entropy perovskite oxides with B-site valence fluctuations for excellent OER performance electrocatalysts

Shibo Wu,Jingrui Cao,Yang Zhou,Jiahao He,Jiangjie Zhou,Muslum Demir,Hongye Yang,Zaizai Tong,Pianpian Ma

High-entropy perovskite oxides, an emerging electrocatalytic electrode material, integrates the distinctive features of high-entropy materials and perovskites, offering significant potential in electrocatalysis. While adjusting the B-site elements has been a widely adopted approach for modulating the electrocatalytic activity of HEPs, there was a notable lack of systematic investigations into the role of A-site ions in regulating their electrocatalytic performance. To overcome this deficiency, in the present study, La 1-x Na x (CrMnFeCoNi) 1/5 O 3 HEPs were synthesized using carbon nanotubes-based sacrificial template method. It was found that the Na substitution at the A-site not only significantly reduced the synthesis temperature but also facilitated the preservation of carbon nanotubes. This retention contributed to the formation of a three-dimensional network structure, exposing a greater number of active sites. The Na modification induced significant valence fluctuations at the B-site and tailored the oxygen vacancy concentrations, enhancing the synergistic "cocktail effect" among the various metal atoms. Furthermore, the introduction of Na stimulated the formation of surface M-OOH species, which serve as active intermediates to enhance OER activity. As a result, the Na-modified HEPs demonstrated exceptional OER performance compared to their parent phases. Among these, La 0.6 Na 0.4 (CrMnFeCoNi) 1/5 O 3 (L6N4-5M) sample exhibited a lower overpotential of 313 mV at a current density of 10 mA cm −2 and a Tafel slope of 47.4 mV dec −1 . Additionally, the A-site Na modification strategy and the in-depth investigation of the OER mechanism provide valuable insights for the future design and development of high-performance HEP electrocatalysts.

研究领域: 材料科学 · 电催化领域
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CHEMISTRY-A EUROPEAN JOURNAL · 2019 ·Vol. 26 ·期 6 ·1306-1313 · IF 5.16

ZnO-Templated Selenized and Phosphorized Cobalt-Nickel Oxide Microcubes as Rapid Alkaline Water Oxidation Electrocatalysts

Muhammad Sohail Riaz,Siwei Zhao,Chenlong Dong,Shuying Nong,Yantao Zhao,Muhammad Javed Iqbal,Fuqiang Huang

Graphical Selenized and phosphorized cobalt-nickel oxide microcubes formed by a novel strategy using a sacrificial ZnO spherical template are employed as an oxygen evolution reaction (OER) electrocatalyst. The selenized samples manifest desirable and robust OER performance, with comparable overpotential at 10 mA cm −2 (312 mV) as RuO 2 (308 mV) and better activity when the current reaches 13.7 mA cm −2 . Oxygen electrocatalysis is of remarkable significance for electrochemical energy storage and conversion technologies, together with fuel cells, metal-air batteries, and water splitting devices. Substituting noble metal-based electrocatalysts by decidedly effective and low-cost metal-based oxygen electrocatalysts is imperative for the commercial application of these technologies. Herein, a novel strategy is presented to fabricate selenized and phosphorized porous cobalt-nickel oxide microcubes by using a sacrificial ZnO spherical template and the resulting microcubes are employed as an oxygen evolution reaction (OER) electrocatalyst. The selenized samples manifest desirable and robust OER performance, with comparable overpotential at 10 mA cm −2 (312 mV) as RuO 2 (308 mV) and better activity when the current reaches 13.7 mA cm −2 . The phosphorized samples exhibit core–shell structure with low-crystalline oxides inside amorphous phosphides, which ensures superior activity than RuO 2 with the same overpotential (at 10 mA cm −2 ) yet lower Tafel slope. Such a surface doping method possibly will provide inspiration for engineering electrocatalysts applied in water oxidation.

研究领域: 材料科学 · 电化学 · 能源存储与转换 · 催化
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APPLIED SURFACE SCIENCE · 2024 · IF 6.3

Directional movement of electron induced by interfacial coupling in CuS@NiCo-LDHs for efficient alkaline oxygen evolution reaction

Li Liu,Jing Mo,Jie Xu,Yangxi Liu,Ruoxi Yang,Xiaohui Yang,Xinguo Ma,Wensheng Fu

Heterojunction has the characteristics of adjusting catalyst structure, improving oxygen evolution kinetics and breaking the elevated reaction barrier of oxygen evolution process. In this paper, a heterostructure catalyst of NiCo-LDHs nanosheets encapsulated CuS hollow nano-octahedrals has been reported, which has better stability and higher mass transfer efficiency compared with two-dimensional nanosheets. Density functional theory (DFT) calculations indicate that the heterostructure strengthens the orbital hybridization of metal 3 d and O 2 p , at the same time, the heterointerface coupling induces the directional movement of electrons from NiCo-LDHs to CuS, which together provide abundant high-valence Ni and Co active sites, promote the conversion of *OH to *O species, thus reducing the energy required for the reaction. Hence, CuS@NiCo-LDHs exhibits excellent OER performance and good stability in 1 M KOH. When the current density is 10 mA/cm 2 , the overpotential and Tafel slope of this catalyst is only 253 mV and 56 mV/dec, respectively. This study furnishes the construction of heterogeneous structures and the catalyst exploitation with serviceable insights.

CAS / MDL: 12036-10-1
研究领域: 催化 · 材料科学 · 电化学 · 纳米技术
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