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Inorganic Chemistry Frontiers · 2024 · IF 6.1

Fabrication of amorphous subnanometric palladium nanostructures on metallic transition metal dichalcogenides for efficient hydrogen evolution reaction

Liang Mei,Yuefeng Zhang,Zimeng Ye,Ting Han,Honglu Hu,Ruijie Yang,Ting Ying,Weikang Zheng,Ruixin Yan,Yue Zhang,Zhenbin Wang,Zhiyuan Zeng

Fabricating solution-processable composite materials of transition metal dichalcogenides (TMDs) with ultrasmall noble metal structures employing an easy preparation method poses a significant challenge. In this study, we utilized a green, one-step synthetic method by directly employing electrochemical lithium intercalation-based exfoliated metallic TMD nanosheets (MoS2, WS2, and TiS2) to reduce palladium ions (Pd2+) to metallic Pd0, leading to the deposition on their surfaces. The resulting Pd nanoparticles (Pd NPs) in composites (Pd-MoS2, Pd-WS2, and Pd-TiS2) were found to be amorphous, with a size ranging from 0.81 to 1.37 nm. The impact of Pd NP size on hydrogen evolution reaction (HER) activity was elucidated. Among the fabricated composites, Pd-MoS2 exhibits the best HER performance, attributed to its smallest Pd NP size (0.81 nm). It shows an overpotential of 70 mV at a current density of 10 mA cm−2, along with a Tafel slope of 43 mV dec−1. These HER performance metrics surpass those of most Pd-decorated 2D catalysts.

研究领域: 材料科学 · 纳米技术 · 电化学 · 催化
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CHINESE CHEMICAL LETTERS · 2019 · IF 3.839

Layered MoS2@graphene functionalized with nitrogen-doped graphene quantum dots as an enhanced electrochemical hydrogen evolution catalyst

Tong Guo,Lina Wang,Sen Sun,Yan Wang,Xiaoling Chen,Kangning Zhang,Dongxia Zhang,Zhonghua Xue,Xibin Zhou

A novel three-dimensional (3D) layered MoS 2 @graphene functionalized with nitrogen-doped graphene quantum dots (MoS 2 @N-GQDs-GR) composites as an enhanced electrochemical hydrogen evolution catalyst. The few layered MoS 2 nanoflowers supported on N-GQDs-GR surface were elaborately fabricated by one-pot hydrothermal method, which MoS 2 and N-GQDs-GR exist in a bonding manner of Mo-N. In addition, due to the layered MoS 2 sheet edge exposes more hydrogen evolution active sites and N-GQDs-GR have high conductivity, the composites exhibit prominent electrocatalytic activity with a low overpotential 99 mV, a small Tafel slope 49.3 mV/dec. Therefore, that the current work will develop HER catalysts may replace Pt.

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

Construction of Ru/NiMoOx@NC with multi-interfacial core-shell structures for urea-assisted hydrogen production

Jingwen Ma,Ruiting Wang,Tianai Zhang,Ying Tian,Jinhao Liu,Junbin Li

Urea-assisted hydrogen production is an emerging hydrogen production technology that offers a new approach to the efficient and clean production of hydrogen energy. The low energy consumption urea oxidation reaction replaces the high energy consumption oxygen evolution reaction (OER), significantly reducing the energy consumption of hydrogen production and achieving the resource utilization of pollutants in wastewater (including urea). It is expected to become an important pathway for green hydrogen production with both economic and environmental benefits. The novel composite catalyst Ru/NiMoOx@NC, prepared by supporting ruthenium on a nitrogen-doped carbon-coated nickel-molybdenum oxide support, exhibits highly efficient bifunctional catalytic activity, enabling it to efficiently catalyze the hydrogen evolution reaction (HER) and promote the urea oxidation reaction (UOR). Specifically, the introduction of trace ruthenium synergizes with the nickel-molybdenum bimetallic oxide to accelerate H 2 generation. The nitrogen-doped carbon substrate enhances the catalyst's electrical conductivity. Additionally, the incorporation of Mo reduces CO poisoning of Ni active sites during the UOR, further to enhance the catalyst's stability. By varying the loading of Ru, materials with optimal and superior properties are obtained. The Ru/NiMoO x @NC catalysts demonstrate excellent UOR (1.37 V vs. RHE@25 mA cm −2 ; 1.39 V vs. RHE@100 mA cm −2 ) and HER (−98 mV@25 mA cm −2 ) performance under alkaline conditions. The current density of the Ru/NiMoOx@NC electrode remains almost unchanged after cyclic voltammetry (CV) tests and chronoamperometric durability tests, exhibiting excellent catalytic stability. In this system, Ru/NiMoOx@NC serves as both the anode and cathode of the urea-assisted hydrogen production battery, which only requires a voltage of 1.56 V to achieve an output current density of 50 mA cm −2 and demonstrates excellent overall water electrolysis stability. This work provides new insights for the design of bifunctional catalysts for urea-assisted hydrogen production.

CAS / MDL: 13478-00-7
研究领域: 能源技术 · 催化 · 材料科学 · 电化学 · 环境科学
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CHINESE JOURNAL OF CATALYSIS · 2025 · IF 17.7

H-incorporated PdRu electrocatalyst for water splitting under alkaline condition

Hao Wu,Xian Jiang,Jingyu Lu,Yibo Li,Xinyan Li,Guidong Ju,Rengui Li,Jing Zhang

The hydrogen evolution reaction (HER) in alkaline water electrolysis faces significant kinetic and thermodynamic challenges that hinder its efficiency and scalability for sustainable hydrogen production. Herein, we employed an in-situ synthesis strategy to incorporate H atoms into the PdRu alloy lattice to form H Inc -PdRu electrocatalyst, thereby modulating its electronic structure and enhancing its alkaline HER performance. We demonstrate that the incorporation of H atoms significantly improves electrocatalytic activity, achieving a remarkably low overpotential of 25 mV at 10 mA cm –2 compared with the Pd, Ru and PdRu catalysts while maintaining robust catalyst stability. Operando spectroscopic analysis indicates that H insertion into the H Inc -PdRu electrocatalyst enhances the availability of H 2 O* at the surface, promoting water dissociation at the active sites. Theoretical calculations proposed that the co-incorporating H and Ru atoms induces s-d orbital coupling within the Pd lattices, effectively weakening hydrogen adsorption strength and optimizing the alkaline HER energetics. This work presents a facile approach for the rational design of bimetallic electrocatalysts for efficient and stable alkaline water electrolysis for renewable hydrogen production.

CAS / MDL: 100-51-6 14898-67-0
研究领域: 电催化 · 氢能 · 材料科学 · 可再生能源 · 物理化学
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ADVANCED FUNCTIONAL MATERIALS · 2024 · IF 18.5

Constructing 2D PtSe2/PtCo Heterojunctions by Partial Selenization for Enhanced Hydrogen Evolution

Bing Hao,Manyuan Gan,Jingjing Guo,Guoshen Li,Yanhui Song,Yongqing Shen,Bingshe Xu,Peizhi Liu,Junjie Guo

The rational design and fabrication of 2D heterojuctions are proven a promising strategy for boosting the performance of electrocatalysts. Although 2D platinum diselenide (PtSe 2 ) exhibits catalytic activity for hydrogen evolution reaction (HER), the catalytic performance is still unsatisfactory due to its inert basal plane, wide bandgap, and poor electron transfer ability. Herein, a new strategy is reported to construct PtSe 2 /PtCo heterojunctions by partial selenization of PtCo alloy for high-efficiency HER electrocatalyst, which exhibits a low overpotential of 38 mV at the current density of 10 mA cm −2 , a small Tafel slope of 22 mV dec −1 , and a superior stability over 24 h and 1000 cycles. The outstanding HER activity of the catalyst arises from the strong electronic interactions between PtSe 2 and PtCo in the heterojunctions, which induce electron transferring from PtSe 2 to PtCo and the d-band center down shifting, and thus optimize the H * adsorption/desorption. This work provides a novel strategy for constructing highly efficient heterostructure electrocatalysts, which facilitates the applications of hydrogen energy conversion.

CAS / MDL: 57-09-0 7782-49-2
研究领域: 材料科学 · 电化学 · 催化
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

Prussian blue analogue-derived CoP nanocubes supported on MXene toward an efficient bifunctional electrode with enhanced overall water splitting

Boyuan Liu,Peng Zhao,Zongdeng Wu,Cai Liu,Haiyan Jing,Juanjuan Song,Keren Lu,Wu Lei,Qingli Hao

The exploration of bifunctional catalyst with economic, durable, and efficient performance plays a crucial role to boost both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in overall water splitting. Herein, we report a feasible strategy to design effective heterostructure between CoP and Ti 3 C 2 T x MXene (denoted as CoP/Ti 3 C 2 T x ). This approach allows for the growth of CoP nanoparticles with uniform size of 5 nm on the Ti 3 C 2 T x MXene, further enhancing the water electrolysis efficiency. The CoP/Ti 3 C 2 T x bifunctional catalyst demonstrates an exceptional HER activity with a satisfactory overpotential of 103 mV at 10 mA cm −2 , and also can drive 10 mA cm −2 for OER with the overpotential of 312 mV in 1.0 M KOH. Moreover, the CoP/Ti 3 C 2 T x -based electrolyzer exhibits high electrochemical stability for 24 h with a low required voltage of 1.66 V at 10 mA cm −2 . The density functional theory (DFT) calculations reveal that the introduction of Ti 3 C 2 T x MXene significantly adjusts d-band center towards Fermi level and expand total density of states, resulting in great electrical conductivity, enhanced water adsorption, and activation. This study provides an available mode for effective design and construction of non-noble-metal-based dual-functional catalyst toward practical energy conversion.

研究领域: 材料科学 · 电化学 · 能量转换
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Energy & Environmental Science · 2018 ·Vol. 12 ·期 3 ·1000-1007 · IF 30.067

Highly stable single Pt atomic sites anchored on aniline-stacked graphene for hydrogen evolution reaction

Shenghua Ye,Feiyan Luo,Qianling Zhang,Pingyu Zhang,Tingting Xu,Qi Wang,Dongsheng He,Licheng Guo,Yu Zhang,Chuanxin He,Xiaoping Ouyang,Meng Gu,Jianhong Liu,Xueliang Sun

Developing efficient and cost-effective electrocatalysts for hydrogen evolution reaction (HER) is highly desired for the hydrogen economy. In this study, we developed a facile microwave reduction method to synthesize single Pt atoms anchored on aniline-stacked graphene (Pt SASs/AG) with outstanding HER performance. Pt SASs/AG presents excellent HER activity with η = 12 mV at 10 mA cm−2 and a mass current density of 22 400 AgPt−1 at η = 50 mV, which is 46 times higher than that of commercial 20 wt% Pt/C. Moreover, the Pt SASs/AG catalyst is highly active and more stable than Pt/C. X-ray absorption fine spectroscopy and density functional theory calculations demonstrated that the coordination of atomically isolated Pt with the nitrogen of aniline optimized the electronic structure of Pt and the hydrogen adsorption energy, eventually promoting HER activity. This study provides a new avenue for the development of single-atom Pt electrocatalysts with high activity and stability.

CAS / MDL: 62-53-3 18497-13-7
研究领域: 材料科学 · 电化学 · 催化
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Small Methods · 2019 ·Vol. 3 ·期 5 ·1900113 · IF 0

Active Site Identification and Evaluation Criteria of In Situ Grown CoTe and NiTe Nanoarrays for Hydrogen Evolution and Oxygen Evolution Reactions

Liu Yang,Haoxiang Xu,Huibing Liu,Daojian Cheng,Dapeng Cao

Developing efficient non-precious bifunctional electrocatalysts for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) is highly critical for overall water splitting. Herein, vertically aligned CoTe and NiTe nanoarrays are synthesized in situ grown on Ni foams (marked as CoTeNR/NF and NiTeNR/NF) via a facile hydrothermal method, and further explore their catalytic activities for overall water splitting. The CoTeNR/NF catalyst exhibits not only excellent OER performance with a low overpotential of 350 mV to deliver 100 mA cm −2 , but also high HER activity only requiring 202 mV overpotential to yield 10 mA cm −2 in alkaline condition. Moreover, experimental technique and density functional theory are combined together to reveal that the real active sites of CoTeNR/NF for OER are from the in situ generated CoOOHspecies on CoTeNR/NF in the OER process, and also propose a new HER performance evaluation criteria of using H 2 O adsorption energy, H 2 O dissociation barrier, and H 2 /OH − desorption energy as an indicator. The new criteria can satisfactorily evaluate the HER performance of as-synthesized samples, while the traditional one of using H adsorption energy as an indicator fails in the HER performance evaluation of as-synthesized samples. It is expected that the new evaluation criteria can be used as a general criteria to evaluate the HER performance of other electrocatalysts.

CAS / MDL: 1336-21-6
研究领域: 材料科学 · 电化学 · 催化 · 能源材料
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ACS Applied Materials & Interfaces · 2018 · IF 8.097

Nanohybrid of Carbon Quantum Dots/Molybdenum Phosphide Nanoparticle for Efficient Electrochemical Hydrogen Evolution in Alkaline Medium

Linjie Zhang,Yanmei Yang,Muhammad Asad Ziaee,Kanglong Lu,Ruihu Wang

The exploration of highly efficient non-noble metal electrocatalysts for hydrogen evolution reaction (HER) under alkaline conditions is highly imperative but still remains a great challenge. In this work, the nanohybrid of carbon quantum dots and molybdenum phosphide nanoparticle (CQDs/MoP) has been firstly demonstrated as an efficient alkaline HER electrocatalyst. The CQDs/MoP nanohybrid is readily prepared through a charge-directed self-assembly of CQDs with phosphomolybdic acid (H3PMo12O40) at the molecular level, followed by facile phosphatizing at 700 °C. The introduction of CQDs greatly helps to alleviate the agglomeration and surface oxidation of MoP nanoparticles and ensures each MoP nanoparticle to be electronically addressed, thus significantly enhancing the intrinsic catalytic activity of MoP. The optimized CQDs/MoP exhibits high-efficiency synergistic catalysis toward HER in 1 M KOH electrolyte with a low onset potential of −0.08 V and a small Tafel slope of 56 mV dec–1 as well as high durability with negligible current loss for at least 24 h.

CAS / MDL: 7681-53-0
研究领域: 材料科学 · 电化学 · 纳米技术 · 能源材料
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2024 · IF 8.1

Mechanism of MOF-derived Fe-doped TiO2 material enhanced by the AC magnetic field on electrochemical nitrogen reduction reaction (eNRR)

Tong-hui Yang,Song Yue,Wei-wei Gong,Ren-qing Wang,Wei-da Hu,Xiao-pan Liu,Peng-zhao Gao,Hang Qin,Wen-ming Guo,Han-ning Xiao

Electrochemical nitrogen reduction reaction(eNRR) is a promising strategy for ammonia production because of its mild reaction conditions, high theoretical conversion rate, and green pollution. However, the strong stability of N   N triple bond and competitive hydrogen evolution reaction (HER) limit the Faraday efficiency and ammonia conversion of eNRR. In recent years, the structural design of catalysts combined with external field enhancement to enhance the AC magnetic field electrocatalytic reaction has received extensive attention. In this study, an eNRR catalyst ( x Fe-M-TiO 2 ) with a high concentration of oxygen vacancies was constructed by the defect engineering strategy. The ammonia conversion rate of eNRR of 1.5Fe-M-TiO 2 was 7.35 μg h −1 mg cat −1 , and the Faraday efficiency was 22.69 %, which was 2 % higher than that before doping. The spin–orbit coupling effect induced by the AC magnetic field further improved the eNRR activity, in which the Faraday efficiency increased to 52.14 % (increased by 150 %), and the ammonia yield increased to 13.37 μg h −1 mg cat −1 (increased by 5 %). After 80 h of eNRR, the current density of the catalyst became 95 % of the initial current density, and the stability was good. Density functional theory calculation showed that Fe doping did not change the reaction mechanism of eNRR but increased the concentration of oxygen vacancy, resulting in a 0.62 eV decrease in the energy barrier of the first hydrogenation of eNRR, which was conducive to the occurrence of eNRR.

研究领域: 材料科学 · 电化学 · 催化 · 纳米技术 · 环境科学 · 化学工程
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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

Encapsulating dual-phased Mo2C-WC nanocrystals into ultrathin carbon nanosheet assemblies for efficient electrocatalytic hydrogen evolution

Xueting Zhang,Zhenye Zhu,Xiongyi Liang,Fei-Xiang Ma,Jiaheng Zhang,Yuanbo Tan,Zuchen Pan,Yiyang Bo,Chi-Man Lawrence Wu

Mo 2 C and WC are widely considered as promising electrocatalysts for hydrogen evolution reaction (HER) owing to their Pt-like electronic features. Herein, dual-phased Mo 2 C-WC nanocrystals, densely and uniformly confined in ultrathin carbon nanosheet assemblies (abbreviated as Mo 2 C-WC/NCAs), which are possible candidates for high-performance HER electrocatalysts, are fabricated through the in-situ pyrolysis of polymers containing Mo and W. When evaluated as HER electrocatalysts, Mo 2 C-WC/NCAs requires a small overpotential of ~126 mV to drive a current density of 10 mA cm −2 , and low Tafel slopes of 72 mV dec -1 and 59 mV dec -1 in acidic and alkaline media, respectively. In addition, the Mo 2 C-WC/NCAs exhibit robust catalytic stability up to 36 h. The introduction of dual-phased carbide heterostructures can modify the electronic structure and simultaneously facilitate the charge transfer of the catalysts, consistent with the density functional theory (DFT) calculations. This work highlights the in-situ construction of multi-phased hetero-metal carbide heterostructures for high-performance electrocatalysis.

研究领域: 材料科学 · 电化学 · 纳米技术 · 催化
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ACS Sustainable Chemistry & Engineering · 2024 · IF 7.1

Implanting CuNi Alloy into NiVOx for H2 Evolution with Ultralow Overpotential and Highly Selective Formate Production

Ying Wu,Wenhui Fang,Min Li,Yutao Cao,Wei Cui,Zengxi Li,Hong Zhao

Electrochemical upgrading of biomass waste (such as glycerol)-assisted water electrolysis for the production of valuable formate and high-purity hydrogen offers a promising route to develop sustainable and clean sources of energy. Herein, using a simple two-step electrodeposition method to implant CuNi alloy in VOx-doped Ni (NiVOx), we construct a competent, stable, and bifunctional heterogeneous catalyst (CuNi–NiVOx) toward hydrogen evolution reaction (HER) and glycerol electrooxidation reaction (GER). The CuNi–NiVOx electrode presents excellent HER activity with an ultralow overpotential of 8 mV in 1.0 M KOH to deliver a current density of 10 mA cm–2 and high GER activity for selective formate production with high Faradaic efficiency (FE). Moreover, the hybrid electrolytic cell formed by the bifunctional CuNi–NiVOx catalyst was able to reach a current density of 10 mA cm–2 with an ultralow voltage (1.308 V). X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) calculations confirm the existence of electron transfer between the O sites and metal sites and between heterogeneous interfaces, thus optimizing the hydrogen adsorption ability (0.02 eV). This work may provide ideas for the engineering of heterogeneous dual-function electrocatalysts for energy-saving hydrogen production and simultaneous highly selective production of formate.

研究领域: 电化学 · 催化 · 能源材料 · 可再生能源
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