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ACS Applied Nano Materials · 2024 · IF 5.3

Mn-Doped Crystalline Ni3S2/Amorphous MoS2 Core–Shell Nanorods as Bifunctional Electrocatalysts for Highly-Efficient Overall Water Splitting

Shaobo Ye,Zhentao Du,Zhengxiang Cai,Deliu Ou,Haonan Guo,Qiao Liu,Weiyou Yang,Qing Shi

Molybdenum disulfide (MoS2), a typical earth-abundant material, is an excellent candidate for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), which fundamentally rely on the regulation of the morphology and electronic structure of MoS2. Herein, Mn-doped amorphous MoS2 coated on Mn-doped crystalline Ni3S2 nanorods (Mn–Ni3S2@MoS2), rationally designed core–shell nanorods, have been fabricated via a facile one-step hydrothermal method as highly efficient bifunctional activities for HER and OER in alkaline solution. The target electrodes deliver a high current density of 100 mA cm–2 at a low overpotential of 187 and 310 mV for HER and OER, respectively, outperforming most MoS2-based catalysts. Moreover, a water-splitting cell based on the Mn–Ni3S2@MoS2 electrode requires a voltage of 1.45 V to reach a current density of 10 mA cm–2, which is superior to the state-of-the-art one of those based on noble metal Pt/C–NF∥RuO2–NF and non-noble metal catalysts. The overall enhanced bifunctional catalytic performance is mainly attributed to the abundant catalytically active sites provided by the Mn-doped amorphous MoS2 and the fast pathway for electron/proton transfer facilitated by the Mn-doped crystalline Ni3S2 nanorods. The incorporated Mn dopants and assembled Ni3S2/MoS2 heterostructure effectively regulate the electronic structure with redistributed charge within the core–shell Mn–Ni3S2@MoS2 electrode.

CAS / MDL: 12036-10-1
研究领域: 材料科学 · 电化学
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Crafting amorphous VO2–crystalline NiS2 heterostructures as bifunctional electrocatalysts for efficient water splitting: The different cocatalytic function of VO2

Weiliang Zhou,Xiaojie Li,Xuan Li,Jiaxin Shao,Hengpan Yang,Xiaoyan Chai,Qi Hu,Chuanxin He

The rational design of bifunctional electrocatalysts is essential to achieve efficient hydrogen production from water splitting. Here, inspired by cocatalysts widely utilized in photocatalysis , we designed a heterostructure comprising amorphous VO 2 and crystalline NiS 2 , aiming at using VO 2 cocatalyst to boost activity of NiS 2 for both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Intriguingly, we found that VO 2 displayed different co-catalytic function in boosting the OER and HER. Specifically, the VO 2 optimized the binding energy of hydrogen intermediate on NiS 2 and thus improved the HER activity. As for the OER, the amorphous VO 2 was easily dissolved in the KOH electrolyte, resulting in the generation of abundant oxygen vacancies in the in-situ generated active phase of NiOOH from NiS 2 , thereby drastically enhancing the OER activity. Consequently, the obtained VO 2 –NiS 2 @CC displayed excellent performance for overall water splitting, with a low voltage of 1.53 V at 10 mA cm −2 .

研究领域: 材料科学 · 催化化学
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DALTON TRANSACTIONS · 2023 ·Vol. 52 ·期 24 ·8456-8465 · IF 4

Tentacle-like core–shell CoNi2S4/C3N4 bifunctional electrocatalysts for efficient overall alkaline water splitting

Qingfei Li,Nan Li,Mianmian Wu,Guifang Sun,Wenjing Shen,Minghao Shi,Jiangquan Ma

Stable and efficient bifunctional electrocatalysts are of great significance for sustainable energy conversion and human society sustainability. However, conventional electrocatalytic materials tend to exhibit high overpotentials and unsatisfactory chemical activities. Herein, we construct novel CoNi2S4/C3N4 nanowires on a nickel foam (NF) electrode as a bifunctional electrocatalyst for alkaline water splitting by a two-step hydrothermal and thermal annealing process. The prepared CoNi2S4/C3N4 electrocatalyst exhibits superior HER (e.g. 40 mV (ηH210)) and OER (e.g. 110 mV (ηO210)) activities in a 1 M KOH electrolyte, which are much smaller than those of bare NF, Co@NF, NiCoO@NF and most reported materials. Furthermore, the stability test at 10 mA cm−2 for 20 h for the CoNi2S4/C3N4 electrocatalyst shows no obvious decay and proves the excellent stability of CoNi2S4/C3N4. In this work, the unique tentacle-like CoNi2S4/C3N4 nanowire nanostructure leads to minimized interfacial resistance and abundant channels during electrocatalysis. Moreover, comprehensive analysis results show that Ni(Co)OOH active sites, which are beneficial for excellent OER activity, partially form on the surface of CoNi2S4/C3N4 during electrocatalysis. Finally, the CoNi2S4/C3N4∥CoNi2S4/C3N4 two-electrode system is constructed and it exhibits a low-voltage water splitting capability of 1.40 V.

CAS / MDL: 12036-10-1
研究领域: 材料科学 · 电化学 · 能源转换
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

The interfacial synergy of hierarchical FeCoNiP@FeNi-LDH heterojunction for efficient alkaline water splitting

Yi-fan Zhang,Xue-wei Wang,Zi-yu Zheng,Wen-hua Zhang,Xuan Liu,Jia-qian Niu

In response to the growing demand for clean, green, and sustainable energy sources, the development of cost-effective and durable high-activity overall water splitting electrocatalysts is urgently needed. In this study, the heterogeneous structure formed by the combination of FeCoNiP and FeNi-LDH was homogeneously dispersed onto CuO nanowires generated by in-situ oxidation of copper foam as a substrate using an electrodeposition method. This multilevel structure exhibits excellent bifunctional properties as an electrode material in alkaline solutions, for the oxygen evolution reaction (OER) and the hydrogen evolution reaction (HER) only 206 mV and 147 mV overpotentials are needed to achieve a current density of 100 mA cm −2 respectively. Full water electrolysis is thus enabled to take place at such a low cell voltage as 1.64 V to reach the current density of 100 mA cm −2 , which exhibits a long-term stability of 30 h. These improved electrocatalytic performances stem from the construction of multilevel structures. The X-ray photoelectron spectroscopy suggests that strong electron transfer occurs between heterogeneous structures, thus facilitating the OER and HER process. The dispersion of CuO nanowires not only increases the electrochemically active surface areas but also improves the overall hydrophilic and aerophobic properties. This work highlights the positive effect of multilevel structure in the design of more efficient electrocatalysts and provides a reference for the preparation of other low-cost, high-activity bifunctional electrocatalysts.

研究领域: 材料科学 · 电化学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

Archipelago-like oxygen-vacancies-enriched amorphous-crystalline heterointerface for enhanced water splitting

Qingcui Liu,Wenhua Cheng,Weilu Zhang,Zhouliang Tan,Juan Ding,Hongtao Liu,Yudai Huang

Advancing the development of proficient bifunctional water splitting electrocatalysts and deciphering the underlying drivers of their performance are pivotal for accelerating the sustainable hydrogen energy sector. In this study, a novel Fe and P dual-doped cobalt molybdate electrocatalyst (P-FCMO@NF) is engineered in-situ on a nickel foam substrate that induces an archipelago-like amorphous-crystalline heterointerface as well as abundant oxygen vacancies (V O ) on the near-surface, in favor of the electron transport and enhancing the water splitting capability respectively. Consequently, P-FCMO@NF exhibits excellent electrocatalytic performance in 1 M KOH solution. The water splitting device shows an ultra-low work voltage of merely 1.55 V at a current density of 10 mA cm −2 and demonstrates a long-term stability. The correlations between microstructural reconfiguration and sustainable electrocatalytic stability of P-FCMO@NF are deeply explored and verified. The work actually offers valuable insights that form a crucial foundation for the strategic design of innovative bifunctional electrocatalysts.

研究领域: 材料科学 · 能源研究
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

Synergistically coupled CoMo/Fe2O3 electrocatalyst for highly efficient and stable overall water splitting

Huamei Tong,Xinyu Zheng,Mengyue Qi,Di Li,Jianjun Zhu,Deli Jiang

Constructing bifunctional non-precious metal electrocatalysts with advanced industrial value and excellent electrocatalytic performance to achieve efficient overall water splitting is important but difficult. Herein, a heterogeneous electrocatalyst comprising of CoMo alloys anchored Fe 2 O 3 nanosheets was prepared by hydrothermal and electrodeposition methods. The strongly coupled interfaces between the CoMo alloys and Fe 2 O 3 nanosheets promote charge redistribution, which could improve electron transfer efficiency and accelerate reaction kinetics, potentially optimizing reactant adsorption energy. Further density functional theory (DFT) calculations reveal that the construction of CoMo/Fe 2 O 3 /NF heterostructured catalyst facilitates to promote interfacial charge redistribution and enhance charge transfer capacity, thus boosting the catalytic performance. Benefiting from this, the optimal CoMo/Fe 2 O 3 /NF heterostructure demonstrates a minimal overpotential of 71 mV at 10 mA cm −2 for the HER and 266 mV at 50 mA cm −2 for the OER. Remarkably, the catalyst served as a bifunctional electrode for water splitting, resulting in a cell voltage down to 1.5 V at a current density of 10 mA cm −2 . This research provides an effective way for the construction of non-precious iron oxides-based bifunctional electrocatalysts using alloy/metal oxide interfacial engineering strategy.

CAS / MDL: 7440-06-4 12036-10-1
研究领域: 材料科学 · 电化学
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JOURNAL OF SOLID STATE CHEMISTRY · 2025 · IF 3.5

Amorphous/Crystalline NiFeS@Ni0.85Se supported on nickel foam as bifunctional electrocatalysts for efficient water splitting

Hongzhi Wang,Xiangcheng Shen,Weiguo Zhang,Suwei Yao

The synthesis of low-cost transition metal bifunctional electrocatalysts that can replace noble metals is crucial for realizing high efficiency hydrogen production from industrial water splitting. Herein, a novel binder-free amorphous/crystalline NiFeS@Ni 0.85 Se bifunctional electrocatalyst material has been fabricated on nickel foam (NF) via a straightforward two-step electrodeposition method. The electrode features a unique structure in which NiFeS nanosheets of uniform size grow on Ni 0.85 Se microspheres, thus providing more active sites. It exhibits a minimal overpotential of 63 mV at 10 mA cm −2 for hydrogen evolution reaction (HER) and 311 mV at 100 mA cm −2 for oxygen evolution reaction (OER). Impressively, when assembled into an electrolytic cell, the electrocatalyst can reach 10 mA cm −2 at just 1.51 V and remains stable for 220 h. Additionally, at 1.68 V, the catalyst reaches 50 mA cm −2 and maintains stable operation for 140 h, demonstrating outstanding water splitting potential. This paper presents a composite material that combines the crystalline and amorphous states, allowing them to complement each other and jointly promote catalytic performance.

CAS / MDL: 7446-08-4
研究领域: 材料科学 · 电化学
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APPLIED SURFACE SCIENCE · 2021 · IF 6.707

A highly efficient and robust hybrid structure of CoNiN@NiFe LDH for overall water splitting by accelerating hydrogen evolution kinetics on NiFe LDH

Jie Wang,Guicai Lv,Cheng Wang

Hydrogen production by electrochemical overall water splitting is considered as a clean and renewable approach for greener energy. However, the efficiency of water electrolysis suffers from the sluggish kinetics and high overpotential of OER. Although NiFe LDH is regarded as a promising OER catalyst, it faces the problem of poor conductivity, resulting in the limitations of HER performance. Herein, a hybrid nano-architecture of CoNiN@NiFe LDH as a bifunctional electrocatalyst for overall water splitting is fabricated via in-situ electrochemically assembling hierarchical NiFe LDH nanosheets on the surface of CoNiN. CoNiN@NiFe LDH shows excellent activities for OER with the overpotentials of 227 and 291 mV to deliver the current densities of 10 and 100 mA cm −2 , respectively. Moreover, an alkaline electrolyzer with CoNiN@NiFe LDH as anode and cathode requires a cell voltage of 1.63 V to achieve 10 mA cm −2 . In addition, the excellent stability with 100 h towards overall water splitting outperforms most transition metal-based bifunctional electrocatalysts. The superior performance is attributed to the abundant active sites, the strong electronic interaction, and the corresponding metal (oxy)hydroxides species generated by in situ surface reconstruction and phase transformation.

研究领域: 材料科学 · 电化学 · 能源转换
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JOURNAL OF MATERIALS SCIENCE · 2020 ·Vol. 55 ·期 35 ·16625-16640 · IF 3.553

Construction of hierarchical NiFe-LDH/FeCoS2/CFC composites as efficient bifunctional electrocatalysts for hydrogen and oxygen evolution reaction

Zhang Zewu,Zhou Jiamin,Wei Hanlin,Dai Yifan,Li Shijia,Shi Haojun,Xu Gang

Abstract Efficient design and preparation of cost-effective and binder-free bifunctional electrocatalysts to accelerate the hydrogen and oxygen evolution reaction (HER and OER) are critical for overall water splitting. In this work, 3D hierarchical NiFe-LDH/FeCoS 2 /CFC electrodes were synthesized for the first time. The carboxyl groups derived from acid treating promote the homogeneously coated FeCoS 2 on CFC, giving rise to the strongly coupled FeCoS 2 /CFC hybrid. The NiFe-LDH exhibited the vertical growth feature on the FeCoS 2 /CFC composite, which can efficiently expose the active edges sites. Due to unique structure and synergistic effect between the components, the NiFe-LDH/FeCoS 2 /CFC exhibits significant electrocatalytic activity and stability under alkaline environments, with overpotentials of 190 and 308 mV to achieve 10 mA cm −2 for OER and HER, respectively, providing it as a promising electrocatalyst for water splitting reaction. In addition, we deeply studied the synergistic catalytic mechanism of NiFe-LDH/FeCoS 2 /CFC, explaining the reasons leading to the improved catalytic performance of HER and OER. Graphic abstract

CAS / MDL: 57-13-6
研究领域: 材料科学 · 电化学
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APPLIED SURFACE SCIENCE · 2019 · IF 5.155

High-performance bifunctional flower-like Mn-doped Cu7.2S4@NiS2@NiS/NF catalyst for overall water splitting

Yaqiong Gong,Yu Lin,Zhi Yang,Feixiang Jiao,Jinhui Li,Wenfei Wang

The investigation of earth-abundant, durable, and efficient bifunctional electrocatalysts for overall water splitting was critical to future renewable energy systems. Herein, flower-like Mn-doped Cu 7.2 S 4 @NiS 2 @NiS was successfully assembled on 3D nickel foam (NF) substrate via a facile two-step hydrothermal‑sulfuration method (denote as flower-like Mn 2 -CNN/NF). Benefited from unique 3D configuration with firm contact between nanoflowers and Ni foam, flower-like Mn 2 -CNN/NF electrode demonstrated a low overpotential of 252 mV to achieve a current density of 50 mA cm −2 and 24 h-long stability toward oxygen evolution reaction (OER) in 1 M KOH. For hydrogen evolution reaction (HER), a stable current density of 10 mA cm −2 at only an overpotential of 87 mV and a low Tafel slope of 43.7 mV dec −1 were observed. Furthermore, when assembled as electrolyzers on both cathode and anode for stable water splitting, a low cell voltage of 1.514 V was needed for flower-like Mn 2 -CNN/NF to afford the current density of 10 mA cm −2 and distinguished durability for over 46 h was observed, which presented a wide range of possibilities for the development of earth-abundant and high efficient electrode pairs.

研究领域: 材料科学 · 可再生能源 · 电化学
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Small · 2021 ·Vol. 17 ·期 45 ·2102078 · IF 13.281

Iridium in Tungsten Trioxide Matrix as an Efficient Bi-Functional Electrocatalyst for Overall Water Splitting in Acidic Media

Pengsong Li,Xinxuan Duan,Yun Kuang,Xiaoming Sun

Electrocatalytic water splitting in acidic media is a promising strategy for grid scale production of hydrogen using renewable energy, but challenges still exist in the development of advanced catalysts with both high activity and stability. Herein, it is reported that iridium doped tungsten trioxide (Ir-doped WO 3 ) with arrayed structure and confined Ir sites is an efficient and durable bi-functional catalyst for overall acidic water splitting. A low overpotential (258 mV) is required to achieve an oxygen evolution reaction current density of 10 mA cm −2 in 0.5 m H 2 SO 4 solution. Meanwhile, Ir-doped WO 3 processes a similar intrinsic activity to Pt/C toward hydrogen evolution reaction. Overall water splitting using the bi-functional Ir-doped WO 3 catalyst shows low cell voltages of 1.56 and 1.68 V to drive the current densities of 10 and 100 mA cm −2 , respectively, with only 16 mV decay observed after 60 h continuous electrolysis under the current density of 100 mA cm −2 . Structural analysis and density functional theory calculation indicate that the adjusted coordination environment of Ir within the crystalline matrix of WO 3 contributes to the high activity and durability.

CAS / MDL: 7783-03-1
研究领域: 材料科学 · 电化学
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY · 2023 · IF 10.9

Engineering Cu1.96S/Co9S8 with sulfur vacancy and heterostructure as an efficient bifunctional electrocatalyst for water splitting

Yuanhua Xiao,Ya Shen,Dangcheng Su,Shiwei Zhang,Jinlin Yang,Dafeng Yan,Shaoming Fang,Xuezhao Wang

Defect and interface engineering have been recognized as efficient strategies for developing high-performance electrocatalysts. However, it is still challenging to couple defect and interface engineering in transition metal sulfides and understand their dynamic evolution process during electrocatalysis. Herein, we developed one-step pyrolysis of bimetallic sulfide to construct S vacancy-rich Cu 1.96 S/Co 9 S 8 heterostructure by controlling the critical decomposition temperature. The as-synthesized Cu 1.96 S/Co 9 S 8 exhibits excellent bifunctional electrocatalytic performance, with a low overpotential of 99 and 200 mV at 10 mA cm −2 towards hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in 1.0 mol/L KOH electrolyte, respectively. A symmetric two-electrode cell with Cu 1.96 S/Co 9 S 8 delivered a current density of 10 mA cm −2 at a low voltage of 1.43 V and showed long-term stability for 200 h. A series of in/ex-situ techniques revealed that the electrochemical reconfiguration only appeared in the OER process, resulting in the CoOOH/CuO and SO 4 2− species promoting OER performance. Meanwhile, the S vacancy and heterostructure interface in Cu 1.96 S/Co 9 S 8 were proved to optimize the electronic structure and the adsorption of intermediates for HER by density function theory (DFT) simulations. This work provides a promising strategy to construct metal sulfides with rich defects and heterogeneous interfaces and understand their dynamic evolution process for electrochemical storage and conversion devices.

研究领域: 材料科学 · 电化学
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