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International Journal of Minerals Metallurgy and Materials · 2022 ·Vol. 29 ·期 5 ·1120-1131 · IF 3.85

Self-supporting and hierarchically porous NixFe—S/NiFe2O4 heterostructure as a bifunctional electrocatalyst for fluctuating overall water splitting

Yan Wenjing,Zhang Jintao,Lü Aijing,Lu Songle,Zhong Yiwei,Wang Mingyong

Stable non-noble metal bifunctional electrocatalysts are one of the challenges to the fluctuating overall water splitting driven by renewable energy. Herein, a novel self-supporting hierarchically porous Ni x Fe—S/NiFe 2 O 4 heterostructure as bifunctional electrocatalyst was constructed based on porous Ni—Fe electrodeposition on three-dimensional (3D) carbon fiber cloth, in situ oxidation, and chemical sulfuration. Results showed that the Ni x Fe—S/NiFe 2 O 4 heterostructure with a large specific surface area exhibits good bifunctional activity and stability for both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) because of the abundance of active sites, synergistic effect of the heterostructure, superhydrophilic surface, and stable, self-supporting structure. The results further confirmed that the Ni x Fe—S phase in the heterostructure is transformed into metal oxides/hydroxides and Ni 3 S 2 during OER. Compared with the commercial 20wt% Pt/C∥IrO 2 —Ta 2 O 5 electrolyzer, the self-supporting Ni 1/5 Fe—S/NiFe 2 O 4 ∥Ni 1/2 Fe—S/NiFe 2 O 4 electrolyzer exhibits better stability and lower cell voltage in the fluctuating current density range of 10–500 mA/cm 2 . Particularly, the cell voltage of Ni 1/5 Fe—S/NiFe 2 O 4 ∥Ni 1/2 Fe—S/NiFe 2 O 4 is only approximately 3.91 V at an industrial current density of 500 mA/cm 2 , which is lower than that of the 20wt% Pt/C∥IrO 2 —Ta 2 O 5 electrolyzer (i.e., approximately 4.79 V). This work provides a promising strategy to develop excellent bifunctional electrocatalysts for fluctuating overall water splitting.

研究领域: 材料科学 · 电化学 · 可再生能源 · 催化
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ACS Catalysis · 2024 · IF 11.3

2 + 1 > 3: Trimetallic Sites on the Zn-IrP2/FeP Electrode Trigger Synergistic Effect to Activate Industrial-Grade Performance for Hydrazine-Assisted Overall Water Splitting

Xiaoli Sun,Jie Liu,Yunmei Du,Yanru Liu,Wenna Wang,Dehong Chen,Ruiyong Zhang,Lei Wang

Constructing multifunctional electrodes with high metal utilization by a one-step synthesis strategy is a serious challenge. Herein, Zn-IrP2/FeP with dual-functional activity induced by trimetallic sites are constructed by the “one-step phosphorization”. Relevant characterizations and DFT calculations reveal that Ir and Fe act as the HER and HzOR sites, respectively, promoting the overall hydrazine splitting (OHzS) at the industrial-level current. Specially the Zn dopant, as an auxiliary active site for Ir–Fe dual-active sites, optimizes the physical structure, electronic configuration, d-band center, and adsorption intermediate capabilities of the Zn-IrP2/FeP/IF electrode from multiple perspectives. As expected, Zn-IrP2/FeP/IF only requires 223.0 and 382.0 mV to drive the industrial-grade current density of 1 A cm–2 for HER and HzOR, respectively. Notably, the voltage of the OHzS for Zn-IrP2/FeP/IF to reach 500 mA cm–2 is 1.38 V lower than that of the OWS. In summary, trimetallic sites exhibit synergetic electrocatalytic functions and synergistically maximize electrocatalytic efficiency. Moreover, the multiactive site mechanism of the dopant as an auxiliary active site is innovatively proposed in this work. This presents a valuable idea for designing multimetal catalysts with high metal utilization efficiency and in-depth investigation of catalytic mechanisms.

研究领域: 电化学 · 材料科学 · 催化 · 能源转换
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Journal of Environmental Chemical Engineering · 2025 · IF 7.2

Interfacial electronic engineering of carbon nanosphere-confined Ni2P-FeP heterojunctions for water splitting and electro‐Fenton

Neng Chen,Xun Cao,Hongqiang Li,Dedong Jia,Yong Li,Xiaojun He

The water splitting with electro-Fenton (WS-EF) system offers a dual-functional approach for sustainable H 2 production and pollutant degradation, of which the key is to the development of catalysts with high conductivity, multi-active sites, and synergized pathways for hydrogen/oxygen evolution reactions (HER/OER) and EF processes. In this work, we propose a metal-organic framework (MOF)-derived synthesis strategy to construct carbon nanosphere-confined Ni 2 P-FeP heterostructures on nickel foam (Ni 2 P-FeP@C/NF) via in-situ confined growth, carbonization-alloying, and phosphidation strategy. First-principles calculations reveal that the carefully engineered Ni 2 P/FeP interface effectively tubes the metal d-band center, achieving an optimal hydrogen adsorption free energy for HER while precisely regulating *OOH intermediate adsorption for OER. The Ni 2 P-FeP@C/NF exhibits outstanding electrocatalytic performance, achieving low overpotentials of merely 69.5/233 mV for HER/OER, along with a voltage of 1.55 V at a current density of 10 mA cm cm −2 for overall water splitting. When employed in the electro-Fenton system, the heterointerface exhibits multifunctional catalytic properties: it selectively promotes the 2e - oxygen reduction pathway (85 % H 2 O 2 selectivity) and achieves remarkable sulfamethazine degradation (0.28 min −1 kinetic rate, 78 % TOC removal) in the KOH solution. The carbon nanosphere-confined Ni 2 P-FeP heterojunction nanospheres demonstrate exceptional long-term stability for both water electrolysis and electro-Fenton catalysis. This work pioneers interface engineering strategies for coupled hydrogen production-wastewater treatment systems by tuning electronic structure.

研究领域: 材料科学 · 电化学 · 环境科学 · 纳米技术 · 能量转换 · 催化
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CHINESE JOURNAL OF CATALYSIS · 2024 · IF 15.7

Quenching to optimize the crystalline/amorphous ratio of CoPS nanorods for hydrazine-assisted total water decomposition at ampere-level current density

Xiao Chen,Yunmei Du,Yu Yang,Kang Liu,Jinling Zhao,Xiaodan Xia,Lei Wang

ABSTRACT Directional construction of crystalline/amorphous (c/a)-phosphosulfide heterostructures with exceptional intrinsic activity through a facile strategy is challenging. In this study, we synthesized q-CoPS nanorods with a unique c/a-CoPS core-shell heterostructure through the ‘gas-phase phosphorus vulcanization-quenching' treatment. This work also innovatively masters the regulation of the initial quenching temperature to alter the c/a ratio of the CoPS nanorods . Surprisingly, with increasing initial quenching temperature, the area of the amorphous CoPS shell gradually increases. Density functional theory calculations reveal that the Co sites at the c/a-heterointerface, as the difunctional c/a-interface active site, effectively optimize the kinetics of the hydrogen evolution reaction (HER) and hydrazine oxidation reaction (HzOR). As anticipated, q-CoPS/CF requires an overpotential of only 90 mV at a current density of 1000 mA cm –2 for the alkaline HER, which is much lower than that required using the state-of-the-art Pt/C catalyst. Additionally, q-CoPS/CF achieves a current density of 1000 mA cm –2 at only 0.06 V in the HzOR. Overall, this work proposes an efficient strategy for developing a bifunctional electrocatalyst with a unique c/a-heterostructure to address future energy needs.

CAS / MDL: 7704-34-9
研究领域: 材料科学 · 电化学 · 能源材料 · 催化
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Phosphorous and cations boost the electrocatalytic performances of Cu-based compounds for hydrogen/oxygen evolution reactions and overall water-splitting

Qihao Wang,Yingxue Du,Yuecheng Gong,Weiping Xiao,Hongdong Li,Yunmei Du,Guangrui Xu,Zexing Wu,Lei Wang

Developing durable, effective and inexpensive electrocatalysts for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) are crucial for the advancement of water splitting as a solution to the energy shortage. In this study, nanospheres stacked into nanochains are successfully prepared by oxidative corrosive engineering, solvothermal, and following calcination process (Co-Cu 3 P/CF). The unique nanochain structure facilitates growing the specific surface area, thereby exposing plenitude active sites. The introduced phosphorus (P) and Co ions can alter the electronic characteristics of metal phosphides, not only can accelerate the electron transport of the catalysts, but speed up the reaction kinetics. Thus, the prepared Co-Cu 3 P/CF exhibits low overpotentials, with 240/84 mV, in alkaline media for OER/HER to attain 10 mA cm −2 . In alkaline freshwater/seawater, the self-assembled electrolyzer needs only 1.51/1.58 V to achieve 10 mA cm −2 . This work provides an approach for the preparation of high-performing and economical electrocatalysts.

研究领域: 电化学 · 材料科学 · 能源存储与转换
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2023 · IF 9.9

Ultrasmall RuM (Mo, W, Cr) Decorated on Nitrogen-doped Carbon Nanosheet with Strong Metal-support Interactions for Electrocatalytic Hydrogen Generation in Wide pH Range

Huizhen Wang,Pengfei Yang,Dongzheng Liu,Mengzhen Yu,Bowen Zhou,Yubing Zhang,Zhenyu Xiao,Weiping Xiao,Zexing Wu,Lei Wang

Developing efficient electrocatalysts for hydrogen evolution reaction (HER) in full pH range can promote the practical applications of hydrogen energy. In this work, nitrogen doped carbon nanosheets supported RuM (Mo, W, Cr) (RuM/NCN) are prepared through an ultrafast microwave approach. The carbon nanosheet structure coupled with the ultrasmall RuM nanoparticles can expose rich active sites to optimize the catalytic activity. Moreover, the strong metal-support interactions also favor to accelerate the reactions kinetics and improve stability. Thus, the developed RuMo/NCN (RuW/NCN) show excellent HER catalytic activities with overpotentials of 72 (75) mV, 82 (82) mV and 124 (1   1   9) mV to reach current density of 10 mA cm -2 in 1 M KOH, 0.5 M H 2 SO 4 and alkaline seawater , respectively, and also achieve excellent performance in 1 M PBS. This work provides a valid and novel avenue to design efficient electrocatalysts in renewable energy-related fields.

研究领域: 材料科学 · 电化学 · 催化 · 能源材料
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JOURNAL OF ALLOYS AND COMPOUNDS · 2025 · IF 6.3

NiFeCoMoCr high-entropy hydroxides for efficient bifunctional alkaline water splitting and renewable hydrogen storage

Rui Zhu,Jianbing Zang,Mingyue Han,Liang Dong,Xueqing Tian,Fanjia Sun,Renjie Liu,Yanhui Wang

High-entropy materials have gained significant attention in the field of electrocatalysis for water electrolysis due to their adaptable electronic properties and the synergistic effects arising from the presence of multiple components. In this context, high-entropy hydroxides (HEHs) have emerged as a focal point of research, attributed to their layered structures and the excellent oxygen evolution reaction (OER) catalytic activity. Herein, a NiFeCoMoCr-HEH catalyst featuring a nanocrystalline structure was synthesized by a one-step hydrothermal method, resulting in the formation of a three-dimensional hierarchical architecture characterized by grape-shaped microspheres comprising interconnected 2D nanosheets. The catalyst demonstrated remarkable OER performance in alkaline conditions, achieving a minimal overpotential of 271.81 mV for a current density of 100 mA cm −2 and maintaining stability for 55 h. To enhance the hydrogen evolution reaction (HER) activity of the catalyst, a minimal amount of Pt metal was deposited onto the NiFeCoMoCr-HEH surface. The Pt-NiFeCoMoCr-HEH catalyst achieved a HER overpotential of 31.85 mV at 10 mA cm −2 with 24 h durability. Upon integration into a water electrolyzer, the coupled Pt-NiFeCoMoCr-HEH||NiFeCoMoCr-HEH system delivered 50 mA cm −2 at 1.58 V, significantly lower than conventional Pt/C||IrO 2 /C systems (1.67 V). Impressively, the system was successfully powered by solar and wind energy, yielding hydrogen and showcasing its viability for renewable energy storage. This work highlights the promise of HEH-based catalysts in advancing environmentally friendly hydrogen production.

研究领域: 电化学 · 能源材料 · 催化 · 可再生能源 · 纳米技术
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2024 · IF 8.1

Superhydrophilic 3D amorphous/crystalline heterostructure: Nanosheets-assembled CoMoP-FexP/NF as efficient bifunctional electrodes for alkaline water splitting

Jiejie Feng,Changshun Chu,Jianting Liu,Liling Wei,Huayi Li,Jianquan Shen

To push forward the hydrogen energy technology, it is crucial to develop a highly active catalyst for the application of water splitting. Nevertheless, many electrocatalysts suffer from functional limitations, making them unsuitable for both anode and cathode applications. Therefore, the utilization of bifunctional electrocatalysts is necessary to overcome this limitation. In this study, we have reported a bifunctional CoMoP-Fe x P/NF catalyst with favorable electrocatalytic performance toward hydrogen evolution reaction/oxygen evolution reaction (HER/OER). Balanced amorphous/crystalline heterophase endows CoMoP-Fe x P/NF with more exposed active sites. In addition, the superhydrophobic nature of CoMoP-Fe x P/NF helps to improve the contact with electrolyte. Following conditional optimization, CoMoP-Fe x P/NF requires only an overpotential of 85.6 mV to achieve a current density of 10 mA cm −2 for HER, and 249.6 mV for a current density of 20 mA cm −2 for OER. A water-splitting electrolyzer comprising CoMoP-Fe x P/NF requires a low cell voltage of 1.56 V to achieve a current density of 10 mA cm −2 . This study provides valuable insights into designing bifunctional electrocatalysts and replacing noble metallic materials to enhance hydrogen production from water splitting.

CAS / MDL: 10026-22-9 12036-10-1
研究领域: 材料科学 · 电化学 · 能源材料 · 催化
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

One-step electrodeposition synthesis of NiFePS on carbon cloth as self-supported electrodes for electrochemical overall water splitting

Yuwei Gui,Zhetong Liu,Xiangbo Feng,Yufei Jia,Yimeng Zhang,Yongming Zhang,Haiyan Yang,Yi Zhang,Mingyang Li,Liang Liang,Jian-Wen Shi

Electrocatalytic water splitting (EWS) for hydrogen production is considered an ideal strategy for utilizing renewable energy , reducing fossil fuel consumption, and addressing environmental pollution issues. Traditional noble metal electrocatalysts have excellent performance, but their cost is high. Developing efficient, stable, and relatively inexpensive dual functional electrocatalysts is crucial for promoting large-scale EWS hydrogen production processes. Herein, a simple one-step electrodeposition method was used to grow nickel–iron phosphorus-sulfides (NiFePS) on the surface of hydrophilic treated carbon cloth (CC). The resultant NiFePS/CC with a phosphorus to sulfur ratio of 1:4 exhibited the best electrocatalytic performance, requiring only −91 mV and 216 mV overpotentials to generate the current densities of 10 mA·cm −2 in hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), respectively. When it was used as a bifunctional electrocatalyst to overall water splitting (OWS), a voltage of 1.536 V can generate a current density of 10 mA·cm −2 . The excellent electrocatalytic performance can be ascribed to two factors: 1) the CC with excellent conductivity serves as a growth substrate, reducing the impedance of charge transfer from the electrode to the electrolyte and accelerating the electron transfer rate; 2) The large number of ultra-thin nanosheets formed on the surface of the catalyst increase the electrochemical specific surface area , expose more reaction sites, and thus improve the electrocatalytic reaction performance. This work provides a new approach for designing efficient non-noble metal electrocatalysts for water splitting.

CAS / MDL: 10025-77-1 10039-56-2
研究领域: 电化学 · 材料科学 · 能源工程 · 催化 · 可再生能源
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS · 2018 ·Vol. 29 ·期 13 ·10744-10752 · IF 2.324

Facile synthesis of Co-CoOx/N-doped carbon nanotubes hybrids as efficient and bifunctional catalysts for hydrogen and oxygen evolution

Liu Changhai,Wang Ke,Zhang Jin,Zheng Xuerui,Liang Qian,Chen Zhidong

Developing low-cost, efficient, and bifunctional electrocatalysts for both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is an attractive yet challenging task. Herein, we report a novel, simple and one-pot method to fabricate ultrafinely dispersed Co-CoO x nanoparticles encapsulated in a nitrogen doped carbon nanotubes (denoted as Co-CoO x /CN) via an efficient thermal condensation of d -glucosamine hydrochloride, melamine and Co(NO 3 ) 2 ·H 2 O. A well-designed Co-CoO x based hybrid that possesses high activity and excellent durability for the OER and HER in alkaline solution has been fabricated. The catalyst displays good stability for 30,000 s and small Tafel slope of 82 mV per decade for OER and 110 mV per decade for HER. Detailed electrochemical and physical studies indicate that the high OER and HER activity of the hybrid catalyst arises from the strong interaction between Co-based NPs and N-doped carbon nanotubes, and especially the synergistic effect of Co and cobalt oxide.

研究领域: 材料科学 · 电化学 · 纳米技术 · 能量转换 · 催化
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ChemElectroChem · 2016 ·Vol. 4 ·期 2 ·340-344 · IF 3.506

Strongly Coupled 3D Nanohybrids with Ni2P/Carbon Nanosheets as pH-Universal Hydrogen Evolution Reaction Electrocatalysts

Yan Li,Pinwwei Cai,Suqin Ci,Zhenhai Wen

Graphical Hydrogen evolution catalyst : Nanohybrids of Ni 2 P nanofilms on carbon nanosheets show high catalytic activity and excellent stability for the hydrogen evolution reaction in pH-universal electrolyte. A reliable strategy has been developed to prepare Ni 2 P nanofilms on carbon nanosheets (CNS) nanohybrids (Ni 2 P/CNS), which involves the preparation of three-dimensional (3D) CNS followed by in situ growth of Ni 2 P nanofilms on the surface of CNS. The Ni 2 P/CNS nanohybrids possess a robust 3D hierarchical structure, in which the Ni 2 P films are solidly overlaid on the surface of the CNS. The Ni 2 P/CNS nanohybrid was characterized by a variety of techniques, including X-ray diffraction (XRD), electron microscopy, X-ray photoelectron spectroscopy (XPS), etc. A series of electrochemical tests demonstrate the Ni 2 P/CNS nanohybrid shows high catalytic activity and excellent stability towards the hydrogen evolution reaction (HER) in pH-universal electrolyte, that is, in acidic, neutral, and basic media. The outstanding performance for Ni 2 P/CNS is correlated with the synergic effects between Ni 2 P and CNS associated with its unique and robust structure.

研究领域: 材料科学 · 纳米技术 · 电化学 · 能量转换 · 催化
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2022 · IF 5.518

Boron-doped CoSe2 nanowires as high-efficient electrocatalyst for hydrogen evolution reaction

Zhiming Liu,Dazhi Gao,Lina Hu,Hui Liu,Ying Li,Yanming Xue,Fang Liu,Jun Zhang,Chengchun Tang

High activity and stable hydrogen evolution reaction (HER) catalysts have an indispensable influence on hydrogen production . Pyrite cobalt selenide (CoSe 2 ) is considered an excellent non-noble metal compound HER catalyst due to its low price and excellent electrical conductivity . However, the HER catalytic activity of CoSe 2 is still not ideal because of the weak adsorption of hydrogen on its active Co site. The anion introduction can improve the electronic structure of the catalyst and thereby enhance the performance of HER. Here, we report that B-doped CoSe 2 nanomaterials on carbon cloth (B-CoSe 2 /CC) were successfully synthesized. Compared with CoSe 2 , B-CoSe 2 exhibits better HER performance in 1 M KOH. The overpotential of B-CoSe 2 catalyst is only 153 mV at 10 mA cm −2 . Tafel slope of B-CoSe 2 /CC sample is only 85 mV dec −1 . In addition, B-CoSe 2 /CC exhibits perfect long-term durability and cycle stability. Density functional theory (DFT) calculations illustrate that the doping of B improves the intrinsic conductivity of CoSe 2 and optimizes the hydrogen adsorption free energy (ΔG H* ) of Se and Co sites. This work not only proposes a new anion doping strategy to improve the electronic structure of cobalt-based selenides for improved HER performance, but also provides a reference for the screening and design of other transition metal compound HER electrocatalysts .

研究领域: 材料科学 · 电化学 · 催化 · 可再生能源
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