CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yilin Wang,Xiaoli Sun,Yunmei Du,Shuangshuang Li,Mengmeng Wang,Yanru Liu,Lei Wang
Optimizing the electronic structure of Ru by introducing N dopants or O vacancies (V O ) into RuO 2 is expected to be a promising strategy to stimulate the hydrogen evolution reaction (HER) performance. However, it is a challenge to develop a fast and low-energy method to simultaneously achieve the construction of N dopants and V O . This work was the first to optimize the quenching technique for achieving the co-introduction of V O and N in Co-RuO 2 nanosheets (N,Co-RuO 2 -V O ). Related characterizations confirmed that V O and N dopants synergistically optimized the electronic configuration of Ru and the reaction path of alkaline HER. As expected, the mass activity of N,Co-RuO 2 -V O (2208.63 mA m g R u - 1 ) was 8.05-fold that of Pt/C at 100 mV for alkaline HER. Surprisingly, N,Co-RuO 2 -V O required only 148.6 mV to achieve an industrial-grade current density of 1 A cm −2 , which was much lower than the commercial Pt/C catalyst (312 mV). Overall, this work provides an energy-efficient new strategy for the development of Ru-based catalysts with ampere-level currents.
研究领域:
材料科学
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电化学
·
催化
✓ 已验证
产品关联
DOI
高影响因子
Journal of the American Chemical Society
·
2025
·
IF 15.6
Ting Gao,Jie Gu,Changheng Yang,Rui Wang,Chan Wang,Pengfei Zhang,Jiatong Li,Xiaoyan Zheng,Yunmiao Fan,Puheng Yang,Xiufu Hua,Junfeng Hui,Huigang Zhang
Hydrogen is a promising clean energy carrier, yet the high energy demand of water electrolysis limits its widespread adoption. Catalysis is crucial to enhance the efficiency of hydrogen production and lower energy costs. However, conventional catalyst design guided by the d-band theory faces inconsistencies in predicting adsorption behavior, and the oxygen evolution reaction (OER) remains a major efficiency bottleneck. To address these challenges, we developed a strain-engineered Rh single-atom catalyst anchored on curved WS2 supported by carbon nanotubes (RhSA/WS2@CNT) to modulate the electronic structure. The resultant catalyst achieves an ultralow overpotential of 17.4 mV at 10 mA cm–2 for the hydrogen evolution reaction (HER) and a mass activity ∼65 times higher than that of commercial Pt/C. Mechanistic analysis reveals that the H* adsorption trend contradicts d-band theory predictions but is explained by orbital symmetry adaptation, where the strain-modulated dxz orbital plays a major role in governing adsorption energetics. Beyond catalyst design, the HER catalyst was coupled with a photocatalytic iodide oxidation reaction (IOR) to replace the OER and reduce the water-splitting voltage to 0.7 V. This study not only introduces a strain-engineering strategy to optimize single-atom catalysts but also demonstrates a coupled electro-photo system that enhances energy efficiency, offering an alternative approach for sustainable hydrogen production.
研究领域:
材料科学
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催化化学
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能源科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ELECTROCHIMICA ACTA
·
2018
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IF 5.116
Jian Du,Xilong Wang,Chao Li,Xin-Yu Liu,Lin Gu,Han-Pu Liang
Studies on highly effective electrocatalysts for producing hydrogen via electrochemical water splitting is of great significance due to the increasing demand of clean and sustainable hydrogen energy economy. In this work, hollow RhCo nanoparticles with an average diameter of 21 nm were fabricated using the galvanic replacement method in a water-ice bath. Electrochemical evaluation showed that the as-synthesized electrocatalyst exhibited better performance for hydrogen evolution reaction (HER) under acid condition, with a lower overpotential of 28.1 mV at 10 mA cm −2 and a lower Tafel slope of 24 mV dec −1 , in comparison with commercial Rh/C. The better HER performance of the as-prepared hollow Rh nanoparticles could be attributed to the larger surface area than commercial Rh nanoparticles, which could provide more active sites and therefore improve the electrocatalytic performance.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2020
·
IF 6.182
Chao Yu,Zhanfang Cao,Shuang Chen,Shuai Wang,Hong Zhong
Designing of catalysts with high activity and earth abundance which can further enhance the electrocatalytic hydrogen evolution performance so as to improve the hydrogen production efficiency. In this paper, we synthesized 1T-MoSe 2 -Se/MgAl-LDH composites by in-situ hydrothermal reduction method. The high proportion 1T phase (73.73%) of ultra-thin layer 1T-MoSe 2 -Se was obtained by acid dissolution operation, which can be ascribed to the limiting growth effect of MgAl-LDH. Compared to Pure MoSe 2 , it dramatically improved HER catalytic activity. the optimal 1T-MoSe 2 -Se (24 h) exhibits superior HER performance with a small overpotential (122 mV at the current density of 10 mA cm −2 ) and Tafel slope (54 mV dec −1 ) as well as excellent electrochemical stability. The introduction of Se can promote the conductivity of 1T-MoSe 2 -Se catalyst. Moreover, the best electrocatalytic hydrogen evolution performance can be exhibited synergistically only when the optimal match between MoSe 2 and Se is achieved, which are confirmed by XPS analysis and HER test results.
研究领域:
材料科学
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化学工程
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能源科学
✓ 已验证
产品关联
DOI
高影响因子
DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 33
·11631-11637
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IF 4
Yunni Liu,Yinghao Tao,Zhaobing Lu,Jing Teng,Weiju Hao,Jun Lin,Guisheng Li
The electrocatalytic nitrogen reduction reaction (NRR) to ammonia is a promising technology to store renewable energy and mitigate greenhouse gas emissions. However, it usually suffers from low ammonia yield and selectivity because of the lack of efficient electrocatalysts. Herein, we report that the construction of metal phosphide heterojunctions is an efficient strategy for NRR activity enhancement. A CoP–MoP heterojunction electrocatalyst, which is fabricated by a facile NaCl template-assisted strategy, exhibits a favorable ammonia yield rate of 77.8 μg h−1 mgcat−1 (38.9 μg h−1 cm−2) and a high faradaic efficiency of 11.16% at −0.50 V versus the reversible hydrogen electrode. The high NRR electrocatalytic activity can be attributed to the electronic coupling effects and interfacial synergistic effects of CoP and MoP at the heterojunction interface, which accelerates the electron transfer rate. Moreover, Mo doping changes the d-band centers of metal sites on the CoP surface, which is conducive to N2 adsorption and promotes N2* adsorption in the competition of occupying active sites, thus inhibiting the HER. This work manifests the high potential of phosphide electrocatalysts and opens an alternative route toward NRR electrocatalysis.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 30
·16427-16435
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IF 12.732
Xue Zhao,Mai Zheng,Zhenyang Zhang,Yufeng Wang,Yingtang Zhou,Xiaohai Zhou,Haibo Zhang
Electrochemical hydrogen evolution reaction (HER) is a green and convenient way to produce hydrogen with high calorific value and zero environmental pollution, but the precious metal Pt, which catalyzes its efficient operation, faces the dilemma of resource scarcity. Before finding an HER catalyst to replace platinum-based materials, morphology control engineering can achieve high-efficiency hydrogen production with a lower platinum input. Here, we used a supramolecular assembly (host: cucurbituril[7]; guest: closo-[B12H12]2−) with weak reducibility as a carrier to convert Pt4+ into ultrafine and highly dispersed Pt nanoparticles (BOPs@Pt) in situ, and the supported Pt-based catalyst (BC3N@Pt) obtained after pyrolysis had the ability to very efficiently catalyze HER. BC3N@Pt exhibited excellent performance in catalyzing HER in the full pH range. Among them, the overpotentials to achieve a current density of 10 mA cm−2 in the media of pH = 14, pH = 7 and pH = 1 were only 26.1 mV, 38.5 mV and 23.1 mV, respectively, and the corresponding Tafel slopes were as low as 41.59 mV dec−1, 59.05 mV dec−1, and 61.07 mV dec−1, respectively. In terms of mass activity, the rate of HER driven by BC3N@Pt was at least three times than that achieved with the commercial 20 wt% Pt/C. The density functional theory (DFT) calculations verified that B doped on CN changes the local electronic distribution, facilitates water dissociation and hydrogen adsorption, and hence enhances the HER activity. The annealing treatment converts the organic polymer into an inorganic BC3N matrix, which not only accelerates the electron transfer rate in HER, but also ensures the stability of BCN@Pt when catalyzing HER in the entire pH range.
研究领域:
材料科学
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电化学
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理论计算
✓ 已验证
DOI
高影响因子
MOLECULES
·
2024
·Vol. 29
·期 17
·4130
·
IF 4.2
Si-Cheng Zhong,Zhe Cui,Jia Li,Guang-Run Tian,Zhong-Hong Zhou,Hong-Fei Jiao,Jie-Fu Xiong,Li-Chen Wang,Jun Xiang,Fu-Fa Wu,Rong-Da Zhao
The electrocatalytic performance of a Fe65Co10Si12.5B12.5Fe-based compounds toward alkaline hydrogen evolution reaction (HER) is enhanced by dealloying. The dealloying process produced a large number of nanosheets on the surface of NS-Fe65Co10Si12.5B12.5, which greatly increased the specific surface area of the electrode. When the dealloying time is 3 h, the overpotential of NS-Fe65Co10Si12.5B12.5is only 175.1 mV at 1.0 M KOH and 10 mA cm−2, while under the same conditions, the overpotential of Fe65Co10Si12.5B12.5is 215 mV, which is reduced. In addition, dealloying treated electrodes also show better HER performance than un-dealloying treated electrodes. With the increase in Co doping amount, the overpotential of the hydrogen evolution reaction decreases, and the hydrogen evolution activity is the best when the addition amount of Co is 10%. This work not only provides a basic understanding of the relationship between surface activity and the dealloying of HER catalysts, but also paves a new way for doping transition metal elements in Fe-based electrocatalysts working in alkaline media.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
PubMed
高影响因子
Nano Energy
·
2024
·
IF 16.8
Jie Liu,Yunmei Du,Xiaoli Sun,Shuangshuang Li,Yanru Liu,Lei Wang
Developing a simple and effective strategy to optimize the structure of phosphide to stimulate its industrial-scale current density for water decomposition is a great challenge. In this work, the ‘phosphorization-quenching ammonia treatment’ strategy was innovatively proposed to prompt N-doping and the phase transition of phosphide, thereby constructing the unique N-FeNiP/NF-T electrode. As anticipated, the well-designed N-FeNiP/NF-T obtained an industrial current density of 1 A cm −2 at only 282 mV for HER and 307 mV for OER, which is 0.90-fold of Pt/C and 0.52-fold of RuO 2 , respectively. Notably, the density functional theory calculation revealed that the N dopants further optimized the reaction kinetics of the N-Ni 2 P/NiP 2 heterostructure with high OER activity and the N-NiP 2 phase with high HER activity, leading to the maximization of the synergistic effect. Overall, this work provides a novel strategy to induce phase transition to construct efficient heterostructure electrodes with optimal reaction kinetics.
研究领域:
材料科学
·
电化学
·
催化
✓ 已验证
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2020
·
IF 7.632
Haidong Yang,Yang Liu,Yutong Luo,Shiqing Lu,Bitao Su,Jiantai Ma
Electrocatalytic nitrogen reduction reaction (NRR) represents a highly promising process to ammonia synthesis for artificial N2 fixation. However, the yield rate for NH3 production and Faradaic efficiency (FE) are still low, which greatly hinder its widespread applications. Until now, although a variety of catalysts, including single-atom catalysts, have been developed for NRR in the pursuit of suppressing hydrogen evolution reaction (HER) and the corresponding higher FE, the limited NH3 yield rate makes them uncompetitive for the synthesis of ammonia. Herein, we report a Fe single-atom catalyst anchoring on a nitrogen-doped carbon substrate (Fe SAC/N–C) as a highly efficient NRR catalyst. The catalyst achieves a high FE of 39.6% in 0.1 M KOH under room temperature, particularly a dramatically enhanced NH3 yield rate of 53.12 μgNH3 h–1 mgcat–1. The isotopic labeling (15N2) experiment confirms that the NH3 production completely originates from N2 reduction. Meanwhile, theoretical calculations and X-ray fine structure analysis reveal that the Fe–N3 coordination of Fe SAC/N–C is indeed responsible for the suppression of HER, particularly resulting in a maximum activation of NRR intermediates to produce ammonia with a high yield rate.
研究领域:
电催化
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
Frontiers in Chemistry
·
2022
·
IF 5.545
Lei Yuxi,Xiao Xuefeng,Ma Tianpeng,Li Weiyin,Zhang Huan,Ma Chao
Layered transition metal dichalcogenides (TMDs), such as molybdenum ditelluride (MoTe2), have attracted much attention because of their novel structure-related physicochemical properties. In particular, semi-metallic-phase MoTe2 (1T′) is considered as a competitive candidate for low-cost electrocatalysts for water splitting. However, there are few reports on the simple hydrothermal synthesis of MoTe2 nanostructures compared with other layered TMDs. In this study, a facile one-step hydrothermal process was developed for the fabrication of layered MoTe2, in which uniform nanotubes with a few layers of 1T′ MoTe2 were fabricated at a lower temperature for the first time. The as-obtained MoTe2 nanotubes were fully characterized using different techniques, which revealed their structure and indicated the presence of layered 1T′ nanocrystals. The efficient activity of MoTe2 nanotubes for the electrocatalytic hydrogen evolution reaction (HER) in 0.5 M H2SO4 was demonstrated by the small Tafel slope of 54 mV/dec−1 and endurable ability, which is attributed to the abundant active sites and remarkable conductivity of 1T′ MoTe2 with a few-layer feature. This provides a facile method for the design and construction of efficient layered MoTe2 based electrocatalysts.
研究领域:
材料科学
·
电化学
·
纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ELECTROCHIMICA ACTA
·
2024
·
IF 5.5
Shijun Xu,Yi He,Siming Yan,Teng He,Hongjie Li,Yuan Gao,Wen Chen,Jin Yan,Guiyang Wu,Xi Yuan
This article elucidates the synthesis of NiMoO 4 -based catalysts with different arrays and crystal structures, including nanowires (nw), nanoplates (ns), and nanocolumns (nc). Subsequently, a high-temperature phosphorization method was employed to generate the corresponding P-NiMoO 4 catalysts. The study investigates the structural evolution of the catalysts and changes in the active species under operational conditions. Concurrently, density functional theory (DFT) calculations provide a more in-depth description of the HER reaction mechanism, considering d-band centers and adsorption energies. Experimental results demonstrate that phosphorized NiMoO 4 with a nanowire array structure and crystal structures of NiMoO 4 and MoO 3 exhibit the optimal HER performance, displaying superhydrophilic and underwater superaerophobic behaviors. The hydrophilic contact angle is 0°, and the aerophobic contact angle is 156.8° This array electrode achieves a current density of 10 mA·cm −2 at an overpotential as low as 73.97 mV. The experiments indicate that through doping and morphology control engineering, catalytic performance can be further synergistically enhanced, providing a new perspective for preparing HER catalytic electrodes with potential applications.
研究领域:
材料科学
·
催化化学
·
理论计算
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2024
·
IF 2.7
Jianzhi Wang,Hongyi Chen,Hongliang Yu,Wangshu Tang,Yuanhang Wu,Yijie Yang,Yu Luo,Jie Yang,Faquan Yu
Designing efficient and cost-effective nonprecious electrocatalysts for the hydrogen evolution reaction (HER) in alkaline solution still remains a significant challenge. Herein, we fabricated a three-dimensional (3D) transition bimetallic phosphate/reduced graphene oxide grown in situ on a nickel foam (NiCoP@rGO/NF) for the HER in alkaline media. NiCoP@rGO/NF exhibits a unique three-dimensional spherical nanostructure with a large specific surface area and short diffusion path, which are conducive to the transfer of electrons. NiCoP@rGO/NF requires an overpotential of only 94 mV at a current density of 10 mA cm−2, with a low Tafel slope (39 mV dec−1), and demonstrates excellent durability in 1.0 M KOH condition. Our work provides a new idea for designing high-performance HER electrocatalysts, which are highly needed in various practical applications.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）