Journal of Energy Chemistry
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2025
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IF 14.9
Jiayu Xu,Fulin Yang,Xia Guo,Shuli Wang,Ligang Feng
Supported Ru nanoparticles with high utilization are promising for the hydrogen evolution reaction (HER) but the effect of the crystal phase engineering of supports on their performance remains unclear. Here, the impact of the crystal phase of the support on the catalytic activity of Ru was probed by anchoring Ru nanoparticles onto precisely synthesized hexagonal (WO 3 -H), orthorhombic (WO 3 -O), and monoclinic (WO 3 -M) supports followed by thorough evaluation for HER. Among them, WO 3 -H demonstrated superior performance by providing enhanced Ru anchoring and uniform dispersion, maximizing active site availability. A critical finding is the small work function difference (Δ W F ) between Ru and WO 3 -H, which minimizes interfacial charge accumulation and facilitates efficient hydrogen spillover, thereby accelerating HER kinetics. In contrast, WO 3 -O and WO 3 -M exhibited larger Δ W F and less effective Ru dispersion, resulting in a larger hydrogen spillover barrier and suboptimal hydrogen adsorption/desorption dynamics. As a result, Ru/WO 3 -H exhibited the best performance, achieving an overpotential of 43.8 mV at 10 mA cm −2 and a Tafel slope of 49.1 mV dec −1 . This work highlights the critical role of the crystal phase in optimizing the intrinsic catalytic activity of catalysts, offering new insights for designing efficient HER catalysts.
研究领域:
材料科学
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电催化
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Kai Deng,Zilong Lian,Wenxin Wang,Jiabao Yu,Qiqi Mao,Hongjie Yu,Ziqiang Wang,Liang Wang,Hongjing Wang
Despite the fruitful achievements in the development of high-performance catalysts, most of materials still suffer limited HER kinetics and poor durability in harsh acidic media, especially at high current densities . In this work, a Pd nanoparticles/Ir metallene heterojunction structure (Pd/Ir hetero-metallene) were successfully prepared by a facile co-reduction method. The hydrogen spillover bridging H + adsorption/H 2 desorption process occurring at the Pd/Ir interface results in the rate-determining step change to a Tafel step, which accelerates the HER kinetics. The Pd/Ir hetero-metallene has a relatively low Δ G Hads (-0.19 eV), which allows for rapid adsorption of H + and release of H 2 , thus greatly improving the performance of HER. As a result, the Pd/Ir hetero-metallene exhibits remarkable HER performance with ultra-low overpotentials of only 69 and 133 mV to reach 500 and 1000 mA cm −2 , a small Tafel slope of 21 mV dec −1 , and superb stability.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
Science Bulletin
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2025
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IF 21.1
Liangdong Hu,Huiyan Zhang,Zupeng Chen,Nengchao Luo,Lian-Hua Xu,Kai Wu,Longfei Hong,Sheng Chu,Rui Xiao
The Liquid-Sunshine presents a transformative approach for converting biomass into high-value platform chemicals. However, conventional photorefineries suffer from low efficiency and excessive byproduct formation due to the inherent incompatibility between biomass and photocatalysts. Herein, we introduce an innovative tandem oxygen-reforming-photocatalysis (TORP) strategy, which first selectively reforms biomass functional groups before driving photocatalytic C–C bond cleavage to produce high-value platform chemicals (HPCs). The oxygen reforming enhances substrate–catalyst interaction and facilitates selective C–C bond activation, while the formation of a hydrogen-rich surface and associated hydrogen spillover promotes C n −1 radical quenching, thereby improving selectivity and suppressing overoxidation. This TORP strategy leads to a seven-fold increase in xylitol yield (1.3 mmol g −1 h −1 ) with 89% feedstock conversion and provides a robust and efficient approach for biomass valorization and exhibits broad applicability across organic waste and plastic substrates, offering strong potential for industrial deployment.
研究领域:
催化化学
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生物质转化
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可再生能源
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有机化学
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光催化
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绿色化学
✓ 已验证
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
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2025
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IF 8.2
Tingxue Fang,Jiawei Wang,Zongxuan Bai,Yuhao Wang,Nan Wang,Dong Xiang,Kedi Cai
It remains critical and challenging to synthesize non-noble metal catalysts with excellent hydrogen evolution reaction (HER) activity in a wide pH range. High-temperature pyrolysis is one of the main methods for catalyst synthesis but can be time-consuming and leads to agglomeration easily. In view of this, molybdenum carbide and molybdenum nitride composite (MoC@MoN) was prepared via CO2 laser irradiation technology. The catalytic activity of the as-prepared catalysts can be effectively regulated by controlling the usage of Na2MoO4·2H2O and the applied CO2 laser power. In acidic and alkaline media, the as-prepared MoC@MoN requires an overpotential of only 63 mV and 34 mV, respectively, at a current density of 10 mA cm–2 and exhibits considerable electrochemical and structural durability, making it a suitable candidate for hydrogen production in a wide pH range. Theoretical calculations reveal the surface adsorption and desorption properties of reactive hydrogen and confirm the energetically favorable hydrogen spillover on the heterostructured MoC@MoN interface. The construction of the heterostructured interface enhances the activation of H2O* and further decreases the energy barrier of H2O* dissociation, thereby promoting the Volmer step and the H* supply for HER on the MoC@MoN interface. The integration of efficient H* adsorption on MoN and easy desorption on MoC effectively accelerates the Tafel step and hydrogen spillover, resulting in excellent HER performance of MoC@MoN. The strategy presented in this paper may offer a unique and viable approach for designing and synthesizing high-performance, low-cost HER catalysts, applied in a wide pH range.
研究领域:
电化学
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催化
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材料科学
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纳米技术
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表面科学
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能量转换
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Yukun Chang,Guangshun Ran,Xing Cheng,Zicong Yang,Hui Song,Yinquan Zhang,Yanhui Chen,Wenyuan Zhou,Jinshu Wang,Hongyi Li
The mechanistic role of interfacial electron transfer in enabling reversible hydrogen spillover for enhanced hydrogen evolution reaction (HER) kinetics remains fundamentally unexplored. Herein, we report a lattice-matched PtCoNiCuZn/ WC x N 1-x heterostructure electrode, where interfacial electron transfer triggers reversible hydrogen spillover, thereby achieving exceptional HER performance. Advanced characterization reveals coherent and semicoherent interfaces that induce charge redistribution, creating electron-deficient Pt sites with optimally downshifted d-band centers. The electrode exhibits a remarkable mass activity of 4.63 A mgPt −1 , which is 22 times higher than that of commercial Pt/C, and demonstrates exceptional stability for over 300 h at 10 mA cm −2 , attributed to strong metal-support interactions (SMSI). Density functional theory (DFT) calculations confirm a reversible hydrogen spillover mechanism driven by a built-in electric field at the heterojunction. This electric field facilitates *H migration from WCN to the alloy, alleviating hydrogen accumulation on the support and enhancing metal-site desorption, thus accelerating HER kinetics. This study provides critical insights into the role of interfacial electron transfer in hydrogen spillover and establishes a rational design strategy for highly active and stable self-supported electrodes in sustainable hydrogen production.
研究领域:
电化学
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催化化学
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材料科学
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纳米技术
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能量转换
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表面科学
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理论化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
·
IF 21.1
Guoshuai Liu,Shanshan He,Hua Zou,Shijie You
Electrocatalytic hydrodechlorination (EHDC) is a promising approach for decomposing chlorinated organic compounds in water treatment. However, the efficiency of EHDC is constrained by kinetic mismatch between C−Cl bond cleavage and atomic hydrogen (H*) utilization. Herein, we develop a heterostructured Pd-H x WO 3 electrocatalyst with Pd nanoparticles (Pd NPs) anchored on H x WO 3 substrate, which can efficiently decompose 2,4-dichlorophenol (2,4-DCP) by taking advantage of the hydrogen spillover effect. Specifically, the resulting Pd-H x WO 3 electrocatalyst exhibits superior dechlorination rate constant ( k = 1.142 h −1 ) and Faradic efficiency (FE = 10.1 %) than monometallic Pd ( k = 0.3600 h −1 , FE = 3.74 %) and bare H x WO 3 ( k = 0.1167 h −1 , FE = 2.11 %), along with exceptional pH adaptability and stability. Electron spin resonance (ESR) and electrochemical and kinetic isotope effect (KIE) measurements indicate that the transport of the H* from H x WO 3 to Pd NPs is the key to enhanced EHDC performance. Theoretical studies reveal that the Volmer step of water dissociation to produce H* is more favorable due to lower transition state (TS) energy (0.344 eV) on H x WO 3 than that on Pd (TS = 0.532 eV). Furthermore, the interfacial electron redistribution in Pd-H x WO 3 lowers the thermodynamic (Δ G = 0.207 eV) and kinetic (Δ G = 0.239 eV) barriers for H* transfer from the internal site of H x WO 3 to interfacial Pd sites, thereby facilitating the proton-coupled electron transfer (PCET)-mediated EHDC on Pd site. This work provides a new proof-in-concept demonstration for designing hydrogen spillover-integrated electrocatalysts to enhance H* generation-transfer-utilization in EHDC for water decontamination.
研究领域:
环境化学
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电催化
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水净化
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材料科学
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可持续化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）