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APPLIED CATALYSIS B-ENVIRONMENTAL · 2021 · IF 19.503

Metal-organic frameworks derived RuP2 with yolk-shell structure and efficient performance for hydrogen evolution reaction in both acidic and alkaline media

Jiahuan Luo,Jing Wang,Yao Guo,Jiawei Zhu,Huihui Jin,Zhiwei Zhang,Daojun Zhang,Yongsheng Niu,Shaogang Hou,Jimin Du,Daping He,Yuli Xiong,Lei Chen,Shichun Mu,Yunhui Huang

Hydrogen generation from electrical water splitting has become a greatly increasing requirement for energy systems, however, highly effective and durable electrocatalysts towards universal-pH hydrogen evolution reaction (HER) remain a big challenge. Herein, we design and synthesize ruthenium di-phosphide (RuP 2 ) confined in carbon layers (RuP 2 -C) with a unique yolk-shell structure (RuP 2 -C@RuP 2 -C) from MOF . As expected, it not only exceeds the HER activity of Pt catalysts, with very tiny overpotentials at 10 mA cm −2 (9 and 17 mV in 1.0 M KOH and 0.5 M H 2 SO 4 , individually), but also has high stability. Besides, it also exhibits a low overpotential (40 mV) close to Pt catalysts and high stability in 1.0 M PBS, indicating that RuP 2 -C@RuP 2 -C (RPC@RPC) owns outstanding HER performance at all pH values. Density functional theory (DFT) calculation results further unravel that the P-site on the surface of RPC@RPC possesses low hydrogen adsorption energy, beneficial for boosting the HER activity.

研究领域: 材料科学 · 电化学
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Nano Energy · 2018 · IF 13.12

Single-crystalline (FexNi1-x)2P nanosheets with dominant {011¯1¯} facets: Efficient electrocatalysts for hydrogen evolution reaction at all pH values

Wei Zhang,Yihui Zou,Hongli Liu,Shuai Chen,Xin Wang,Huawei Zhang,Xilin She,Dongjiang Yang

Electrocatalytic hydrogen evolution reaction (HER) plays a critical role in developing hydrogen and fuel cell technologies . At present, only platinum (Pt) and its compounds are thought to be efficient electrocatalysts for HER, particularly at all-pH values. However, the scarcity and high cost of Pt-based catalysts have seriously hindered their practical application in HER. Here, we report a two-step method for synthesizing single-crystalline (Fe x Ni 1-x ) 2 P nanosheets with exposed { 01 1 ¯ 1 ¯ } facets on Ni foam. Compared with pristine Ni 2 P, the (Fe x Ni 1-x ) 2 P nanosheets exhibit a dramatically improved HER activity (an overpotential of 81, 90, 103 mV at 10 mA cm −2 in acidic, neutral and alkaline media , respectively). Based on the density functional theory (DFT) calculations, it is observed that trace Fe-doping can lead to more charge accumulation around P active sites, which accordingly decreases the Δ G H* and Δ G H2O and promotes the catalytic activity .

CAS / MDL: 12125-01-8
研究领域: 材料科学 · 能源科学
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Journal of Materials Chemistry A · 2024 · IF 10.7

Interfacial electron-engineered tungsten oxynitride interconnected rhodium layer for highly efficient all-pH-value hydrogen production

Ben Zhang,Yijuan Zheng,Zhenyu Xing,Zihe Wu,Chong Cheng,Tian Ma,Shuang Li

Designing and synthesizing eco-friendly and efficient catalysts for the hydrogen evolution reaction (HER) plays a crucial role in the field of large-scale and high-purity hydrogen production. However, it is severely hampered by the sluggish kinetics of the water dissociation step in non-acidic media. To optimize catalytic kinetics, interfacial electron engineering between active sites and supports has been regarded as an essential strategy to achieve compelling electrocatalytic all-pH-value-hydrogen production. Herein, we present the successful fabrication of WNO-coupled Rh layers (Rh–WNO) by a simple thermal treatment of a urea sol–gel with mixed W and Rh salts. This facile one-pot synthetic method is easy to scale up and the resulting Rh–WNO catalyst features Rh nanoclusters anchored on the surface of the well-ordered WNO crystals via Rh–N and Rh–O bonds. The optimal catalyst, Rh–WNO, delivered low overpotentials of 19, 22, and 134 mV at a current density of 10 mA cm−2 in 0.5 M H2SO4, 1.0 M KOH, and 1.0 M PBS, respectively. Notably, Rh–WNO exhibits a high turnover frequency (TOF) of 7.84 H2 s−1 in alkaline conditions, which is much higher than those of Pt/C (0.9 H2 s−1), Rh/C (0.77 H2 s−1), and most of the reported HER electrocatalysts. This work may provide an effective and economic approach for scaling up the production of highly efficient and stable metal nitride-based HER catalysts.

研究领域: 材料科学 · 能源化学
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Journal of Materials Chemistry A · 2018 ·Vol. 6 ·期 44 ·21969-21977 · IF 9.931

Solid-phase hot-pressing synthesis of POMOFs on carbon cloth and derived phosphides for all pH value hydrogen evolution

Yu-Jia Tang,Yifa Chen,Hong-Jing Zhu,A.-Man Zhang,Xiao-Li Wang,Long-Zhang Dong,Shun-Li Li,Qiang Xu,Ya-Qian Lan

Designing an all pH value hydrogen evolution reaction (HER) electrocatalyst with low cost and high activity is urgently needed for future energy storage and conversion systems. Metal–organic frameworks (MOFs) with well-defined pore structures and various metal sources provide feasible platforms for the design of efficient electrocatalysts. However, MOFs as crystalline materials are mostly in crystal or powder form, which would hinder their practical application. Herein, polyoxometalate-based MOFs (POMOFs) were synthesized on carbon cloth (CC) through a facile and general solid-phase hot-pressing method for the first time. The thus-obtained POMOFs/CC can be converted into three phase bimetallic phosphides coated with porous carbon on CC through a phosphidation process, show high electrocatalytic stability over a wide pH range (pH, 0–14) and possess excellent HER performance with low overpotential (e.g., 90.5 mV at 10 mA cm−2 in 1 M KOH). Moreover, the POMOFs/CC derived phosphides present high selectivity for H2 production (nearly 100% faradaic efficiency) and ultra-low charge-transfer resistance (0.96 Ω) in alkaline medium, which hold promise for practical applications. This work provides a powerful strategy for the facile production of fast nucleating MOF-derived electrodes with potential for industrial-scale application in energy storage and conversion.

研究领域: 材料科学 · 能源化学
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