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JOURNAL OF ALLOYS AND COMPOUNDS · 2025 · IF 6.3

A scalable synthesis strategy for Mott-Schottky heterojunction with Ni3S2 as a self-supporting template for boosting OER/MOR

Xiaomin Lang,Juan Huang,Mochou Zhang,Zitao Liu,Chunmei Li,Jianfeng Tang,Qing Li,Hua Lin

Building Mott-Schottky heterojunctions can effectively enhance the activity of catalysts, but it faces challenges such as energy band matching, interface contact quality, and charge transfer efficiency. This study utilizes Ni 3 S 2 as a self-supporting template to construct CoFeLDH/Ni 3 S 2 /NF with a Mott-Schottky heterojunction, which exhibits excellent bifunctional catalytic activity and stability, achieving overpotentials of 227   mV and 107   mV for 10   mA   cm -2 in OER and MOR, respectively. The research indicates that the robust Mott-Schottky interaction established between the metallic Ni 3 S 2 and the semiconductor CoFeLDH promotes spontaneous electron transfer and regulates the adsorption/desorption of intermediates; the Ni 3 S 2 nanosheet array morphology provides a low-resistance pathway for charge and mass transfer, while the small nanosheets of CoFeLDH combined with Ni 3 S 2 enhance the exposure of active sites, further increasing the reaction rate. This strategy can be extended to other semiconductor materials, as demonstrated by the constructed NiFeLDH/Ni 3 S 2 /NF and NiCoLDH/Ni 3 S 2 /NF, which also exhibit good catalytic performance. This study proposes a universal method for constructing efficient Mott-Schottky electrocatalysts, highlighting their practical application potential.

研究领域: 材料科学 · 电化学 · 催化科学
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2021 · IF 5.816

N-doped hollow porous carbon spheres@Co Cu Fe alloy nanospheres as novel non-precious metal electrocatalysts for HER and OER

Jiaxian Liu,Guyang Ning,Kun Shi,Man Zheng,Yuena Sun,Yongjun Gao,Yufan Zhang,Huan Wang

In this work, a string of different proportion trimetallic loaded the N-doped hollow porous carbon nanospheres (N-HPCS@Co Cu Fe NSs) were successfully crafted by a simple and economical method. Herein, the hollow-carbon structure was formed by etching carbon nanospheres. Moreover, owing to the presence of the PDA and P123, high dispersed nano spheres with mesopores were obtained. By this way, the catalyst can expose unique internal cavity and short transport path. Meanwhile, trimetal-based metal-organic frameworks (MOFs) Co Cu Fe alloy nano spheres (Co Cu Fe NSs) are first prepared. Creatively, PDA acts as the carbon resource, nitrogen resource and metal grafting agent simultaneously. Through a series of tests, N-HPCS@Co 1 Cu 1 Fe NSs has the best electrocatalytic performance and durable stability. This work highlights the current advances of hollow porous carbon structure, trimetallic active sites and N-doping, as well as, endow high electrocatalytic activity and durability for HER and OER .

研究领域: 材料科学 · 电化学
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ACS Applied Materials & Interfaces · 2020 · IF 8.758

Lanthanides Regulated the Amorphization–Crystallization of IrO2 for Outstanding OER Performance

Chenglong Ma,Wei Sun,Waqas Qamar Zaman,Zhenhua Zhou,Hao Zhang,Qicheng Shen,Limei Cao,Ji Yang

Research has been focused on regulating the amorphous surface of Ir-based materials to achieve a higher oxygen evolution reaction (OER) activity. The IrOx amorphous layer is generally considered to be substantial enough to break the limitation created by the conventional adsorbate evolution mechanism (AEM) in acidic media. In this work, we used lanthanides to regulate IrOx amorphization–crystallization through inhibiting the crystallization of iridium atoms in the calcination process. The chosen route created abundant crystalline–amorphous (c-a) interfaces, which greatly enhanced the charge transfer kinetics and the stability of the materials. The mass activity of iridium in the synthesized IrO2@LuIr1–nOx(OH)y structure reached 128.3 A/gIr, which is 14.6-fold that of the benchmark IrO2. All the IrO2@LnIr1–nOx(OH)y (Ln = La–Lu) structures reflected 290–300 mV of overpotential at 10 mA/cmgeo2. We demonstrate that a highly active c-a interface possesses an efficient charge transfer capability and is conducive to the stability of the activated oxygen species. The surface-activated oxygen species and the tensile strain [IrO6] octahedron regulated by lanthanides are synergistically beneficial for increasing the intrinsic OER activity. Our research findings introduce c-a interface generation by the regulation of lanthanides as a new method for the rational design of robust OER catalysts.

研究领域: 材料科学 · 电化学 · 催化
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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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NEW JOURNAL OF CHEMISTRY · 2022 ·Vol. 47 ·期 5 ·2619-2625 · IF 3.925

Boosting the OER activity of amorphous IrOx in acidic medium by tuning its electron structure using lanthanum salt nanosheets

Xuefeng Wang,Haeseong Jang,Zijian Li,Haisen Li,Guangkai Li,Min Gyu Kim,Xuqiang Ji,Qing Qin,Xien Liu

Promoting the activity of Ir-based nanomaterials for oxygen evolution reaction (OER) in acid media without losing their durability is crucial for reducing overpotentials in energy conversion, such as electrochemical water splitting. Here, a nanocomposite composed of a-IrOx and lanthanum salt (LaCO3OH) was constructed to further improve its OER activity by tuning the electronic structure of a-IrOx, because a-IrOx is a well-known critical material as the active layer of Ir-based anodic catalysts. The interaction between Ir and La via O atoms as a bridge in the catalyst IrOx/LaCO3OH, verified by X-ray absorption near edge structure spectroscopy, tunes the electronic structure of a-IrOx and thus obviously enhances its activity for the OER in acid media, compared with commercially available IrO2 as well as most of the reported Ir-based OER electrocatalysts. The overpotential of IrOx/LaCO3OH at a current density of 10 mA cm−2 is 255 mV with a Tafel slope of 55 mV dec−1. This work reveals that the strong electronic interaction between Ir- and La-based materials can efficiently improve activity and reduce energy consumption, as well as enlarging the family of acidic OER electrocatalysts.

研究领域: 材料科学 · 电化学 · 催化 · 能源转换
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JOURNAL OF APPLIED ELECTROCHEMISTRY · 2024 ·Vol. 54 ·期 10 ·2269-2279 · IF 2.4

Modulation in the electronic structure of Ir-rich shell on AuIr solid solution as OER electrocatalyst for PEM electrolyzer

Huang He,Chen Taipu,Fang Dahui,Cao Longsheng,Wang Guoxiang,Hao Jinkai,Shao Zhigang

The design of low-cost and high-performance anodic electrocatalyst is essential in proton exchange membrane water electrolysis (PEMWE) application. Herein, we design and synthesize a core–shell structure with Ir-rich shell and AuIr alloy core by using a simple liquid phase reduction method, which exposed a large number of active sites. The d-band center of Ir active sites, merely 2 nm in size, was shifted by the electronegativity difference between the Au and Ir atoms at the core–shell interface. The strong electronic effect can inhibit the dissolution and corrosion of Ir active sites under acidic and high potential conditions. As a result, Ir x @Au 0.25 Ir 0.75− x catalyst shows merely 235 mV overpotential at the current density of 10 mA cm −2 , 75 mV lower than the commercial Ir black catalyst, and 2.6-fold higher mass activity than the commercial Ir black catalyst. Furthermore, when Ir x @Au 0.25 Ir 0.75− x was used as the anionic catalyst, the electrolysis voltage at 1 A cm −2 is 1.7 V in PEMWE, and this activity was maintained for more than 100 h and had exhibited excellent stability, indicating its ideal prospects as an electrocatalyst. Graphical abstract AuIr alloy with Ir-rich core and AuIr alloy shell exposed numerous active sites and improved the utilization efficiency of electrocatalyst.

研究领域: 电化学 · 材料科学 · 催化 · 纳米技术 · 能量转换
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ACS Applied Materials & Interfaces · 2021 · IF 9.229

Surface Reconstruction for Forming the [IrO6]–[IrO6] Framework: Key Structure for Stable and Activated OER Performance in Acidic Media

Cheng-Long Ma,Zhi-Qiang Wang,Wei Sun,Li-Mei Cao,Xue-Qing Gong,Ji Yang

The surface reconstruction of iridium-based derivatives (AxIryOz) was extensively demonstrated to have an excellent oxygen evolution reaction (OER) performance in an acidic medium. It is urgent to use various spectroscopy and computational methods to explore the electronic state changes in the surface reconstruction process. Herein, the underestimated Lu2Ir2O7 was synthesized and investigated. Four typical forms of electrochemistry impedance spectra involved in the reconstruction process revealed three dominating forms of reconstructed pyrochlore in the OER stage, including the inner intact pyrochlore, mid metastable [IrO6]–[IrO6] framework, and the outer collapse amorphous layer. The enhancing electron transport efficiency of the corner-shared [IrO6]–[IrO6] framework was revealed as a critical role in acidic systems. The density of state (DOS) for the constructed [IrO6]–[IrO6] framework corroborated the enhancement of Ir–O hybridization and the downshift of the d-band center. Additionally, we contrast the pristine and reconstruction properties of the Pr2Ir2O7, Eu2Ir2O7, and Lu2Ir2O7 in alkaline and acidic media. The DOS and the XANES results reveal the scale relationship between the O 2p band center and the intrinsic activity for bulk pyrochlore in alkaline media. The highest O 2p center and the highest Ir–O hybridization of Lu2Ir2O7 exhibited the best OER performance among the Ir-based pyrochlore, up to a ninefold improvement in Ir-mass activity compared to IrO2. Our findings emphasize the electrochemical behavior of the reconstruction process for activated water-splitting performance.

研究领域: 材料科学 · 电化学 · 催化 · 光谱学 · 计算化学
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2025 · IF 8.3

Modulation of the electronic structure of AuIr alloy anchor on vacancy–deficient Nb2O5-x as OER electrocatalyst for PEM water electrolysis

Guoxiang Wang,Taipu Chen,Dahui Fang,Jinkai Hao,Zhigang Shao

The development of highly active and stable catalysts of oxygen evolution reaction (OER) plays a crucial role in proton-exchange-membrane water electrolysis (PEMWE). Herein, an electronic modulate was used to fabricate oxygen defect-rich and supported metal catalysts AuIr/Nb 2 O 5-x , and it promoted the sluggish kinetics and low efficiencies of OER with the interaction between oxygen defects and the active sites. The Nb–O defect with an electron redistribution and manipulated active electronic state tailored the OER performance. The Ir actively exposed the AuIr/Nb 2 O 5-x -500 catalyst, which exhibited a low overpotential of 230 mV and maintained an excellent stability for 200 h at the current density of 10 mA cm −2 in 0.5 M H 2 SO 4 electrolyte. Furthermore, the PEMWE using AuIr/Nb 2 O 5-x -500 as the anode revealed a high water-splitting performance (1.61 V @ 0.5 A cm −2 & 1.70 V @ 1 A cm −2 ). In-situ Raman spectra and theoretical calculations revealed the electronic structure of AuIr/Nb 2 O 5-x -500 and the mechanism of OER processes, which rationalized the improved performance through the synergistic effect of metal–support interaction and defect effect.

CAS / MDL: 107-21-1 21348-59-4
研究领域: 电化学 · 催化 · 材料科学 · 能量转换 · 表面科学
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2024 · IF 8.1

Three-dimensional pine-tree-like bimetallic sulfide with maximally exposed active sites by secondary structural restructuring for efficient electrocatalytic OER

Jianzhi Wang,Yuanhang Wu,Hongliang Yu,Congshu Hang,Wangshu Tang,Yijie Yang,Hongyi Chen,Hui Li,Faquan Yu

Developing efficient, low-cost and bifunctional catalysts with predominant durability for the hydrogen evolution reaction (HER) and the oxygen evolution reaction (OER) is an extraordinary challenge in the preparation of green hydrogen energy by electrochemical water splitting. Three-dimensional (3D) transition metal compounds have become a research hotspot as OER electrocatalysts , which can replace noble metal oxides such as RuO 2 and IrO 2 to reduce application costs. Herein, we synthesized a novel three-dimensional pine-tree-like bimetallic sulfide arrays on nickel foam (FeCoS/NF) using various optimization strategies such as morphology optimization, in situ growth and introduction of heterogeneous structures. The as-synthesized FeCoS/NF electrocatalyst only requires relatively low overpotential of 156 mV to achieve a current density of 20 mA cm −2 for OER, with a Tafel slope of only 37 mV dec −1 . It also has a small charge transfer resistance, an electrochemical surface area and good electrochemical stability in alkaline electrolytes . The excellent performance of FeCoS/NF can be attributed to the synergistic effect and amorphous phase of FeCoS as well as the well-defined pine-tree-like array architecture with a large surface area, abundant active sites, and sufficient gas and electrolyte diffusion channels.

研究领域: 材料科学 · 电化学 · 催化 · 能源材料
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ACS Sustainable Chemistry & Engineering · 2025 · IF 7.3

A Sol–Gel–Hydrothermal Interfacial Regulation Strategy for Sulfate Intercalation in NiFe-LDH to Promote High-Valent Ni Formation and LOM-Type OER

Jinlong Zhang,Yuxiang Jin,Zhiqiang Xu,Yizhi Du,Yawen Xu,Xiaoli Ren,Bing Xue,Daoxin Liu,Yongfu Zhu,Fangfei Li

Modulating the electronic state of nickel is a crucial strategy for activating lattice oxygen participation in the oxygen evolution reaction (OER). Herein, a sol–gel-assisted hydrothermal strategy is employed to synthesize sulfate-intercalated NiFe-LDH (SG-S-NiFe-LDH), where SO42– anions are stably incorporated into the interlayer galleries to modulate Ni oxidation states. This interfacial regulation reconstructs the local electronic environment, enabling the formation of high-valent Ni species and favoring a lattice-oxygen-mediated (LOM) pathway. Structural characterizations confirm successful anion incorporation, while post-OER XPS evidences Ni3+/Ni4+ enrichment. Mechanistic studies, including pH-dependent kinetics and O–O intermediate trapping, further validate LOM dominance. SG-S-NiFe-LDH exhibits outstanding activity with a low overpotential of 177 mV at 10 mA cm–2, a Tafel slope of 32.98 mV dec–1, and long-term durability exceeding 170 h. Post-OER HRTEM and ICP confirm structural robustness and minimal Ni loss. Density functional theory calculations reveal that sulfate intercalation raises the Ni d-band center, strengthens *OOH adsorption, and reduces the *OOH → *OO barrier to 0.53 eV. Moreover, a water-splitting device using SG-S-NiFe-LDH as the anode achieves 100 mA cm–2 at 1.66 V with stable 28 h operation. Faradaic efficiency above 98% with an O2:H2 ratio of 1:2 confirms high reaction selectivity. This work demonstrates a targeted anion intercalation strategy to modulate transition-metal states, unlock lattice oxygen reactivity, and advance efficient and durable water electrolysis.

研究领域: 电化学 · 材料科学 · 催化 · 纳米技术 · 能量转换 · 表面科学 · 理论化学
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ACS Catalysis · 2024 · IF 11.3

Grain Boundary-Derived Local Amorphization Enhances Acidic OER

Mingze Sun,Helai Huang,Xiangfu Niu,Shuyan Gong,Zhengwen Li,Jinjie Fang,Xiang Liu,Yanjun Chen,Haohong Duan,Zhongbin Zhuang,Satoshi Nagao,Yuki Aoki,Liang Zhang,Zhiqiang Niu

IrOx of the amorphous phase has long been recognized to exhibit higher catalytic activity than crystalline analogues toward oxygen evolution reaction (OER) but always at the expense of reduced stability. Here, we report an ultrathin Ir surface with high-density grain boundaries (GBs), which transforms into locally stabilized amorphous IrOx by forming an Ir/IrOx interface under OER conditions. The catalyst displays a low overpotential of 263 mV at 10 mA cm–2 and a mass activity (5.8 A mgIr–1 at 1.53 V) of over 90-fold higher than that of commercial IrO2, along with long-term stability for over 350 h. The activity enhancement arises from the stronger binding strength of *OOH on the amorphous GBs relative to the crystalline region, thus breaking the scaling relationship between *OH and *OOH and reducing the energy barrier for the potential determining step of the OER. Proton exchange membrane water electrolysis using this catalyst achieves 2.7 A cm–2 at 2 V cell voltage and operates stably at 1 A cm–2 for over 200 h. The stabilization of the amorphous IrOx phase at GBs may accelerate the development of more active and robust acidic OER electrocatalysts.

CAS / MDL: 3264-82-2
研究领域: 材料科学 · 电化学
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PHYSICA STATUS SOLIDI A-APPLICATIONS AND MATERIALS SCIENCE · 2021 ·Vol. 218 ·期 22 ·2100377 · IF 1.981

2D Nanosheets of Mo2C/CoMoS4 as Active Electrocatalyst for Water Splitting

Pan Liu,Sumin Wang,Yufei Quan,Zhiruo Shen,Qiguan Wang

2D composited nanosheets of Mo 2 C/CoMoS 4 are synthesized by a hydrothermal approach to obtain a bifunctional water-splitting electrocatalyst for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in aqueous alkaline solution. Due to the richened defects formed on the 2D catalyst, the as-derived Mo 2 C/CoMoS 4 exhibits high activity. At 10 mA cm −2 , the HER and OER overpotentials of the 2D Mo 2 C/CoMoS 4 nanosheets are just 117 and 250 mV, respectively, with the corresponding Tafel slope of 90 and 75 mV dec −1 , near to the commercial Pt/C and IrO 2 . X-ray photoelectron spectroscopy proves the strong interactions between Mo 2 C and CoMoS 4 and the Raman analysis certifies the presence of richened defects in Mo 2 C/CoMoS 4 . Moreover, the Mo 2 C/CoMoS 4 possesses a long-term catalytic stability, showing potential application in the water splitting.

CAS / MDL: 15060-55-6 25155-30-0
研究领域: 材料科学 · 电化学
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