Vandung Dao , Hyuk Choi , Sunny Yadav , Juan D. Jiménez , Chiyeop Kim , Tuan Van Nguyen , Kai Chen , Periyayya Uthirakumar , Quyet Van Le , Sanjaya D. Senanayake , Hyun You Kim , In-Hwan Lee
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引用次数: 0
摘要
基于氢溢出效应，多功能二元催化剂在碱性析氢反应中具有广阔的应用前景。其中一个位点可以吸附和解离水，而邻近的位点有利于释放氢。受这些可能性的启发，合成了富氧空位(Ov)的LaCeOx偶联n掺杂石墨烯/Ru单原子(LaCeOx @NGr/Ru1)作为高效的双位点HER催化剂。在碱性介质中，在电流密度为10 mA cm−2的情况下，其过电位为22 mV，塔菲尔斜率为40 mV dec−1，优于先进的钌基催化剂。此外，这种有前途的二元组分催化剂比商用Pt/C催化剂(20% wt%)具有更高的质量活性和更长的持久耐用性。实验和理论研究基于三个必不可少的步骤:水在富含ov的LaCeOx上的吸附和解离，生成的H*向Ce3+-N-Ru1桥的扩散，以及Ru1位点上的氢演化，为LaCeOx @NGr/Ru1的HER机制提供了深入的见解。
LaCeOx coupled N-doped graphene/Ru single-atoms as a binary-site catalyst for efficient hydrogen evolution based on hydrogen spillover
Based on the hydrogen spillover effect, versatile binary-site catalysts are promising for the alkaline hydrogen evolution reaction (HER). In which one site can adsorb and dissociate water, while the neighboring site is favorable for liberating hydrogen. Inspired by these possibilities, oxygen vacancy (Ov)-rich LaCeOx coupled N-doped graphene/Ru single-atoms (LaCeOx @NGr/Ru1) was synthesized as an efficient dual-site HER catalyst. It delivered an impressive low overpotential of 22 mV at a current density of 10 mA cm−2 and a slight Tafel slope of 40 mV dec−1 in an alkaline medium, outstanding the advanced Ru-based catalysts. Moreover, this promising binary-component catalyst exhibited higher mass activity and longer lasting durability than commercial Pt/C catalyst (20 wt%). Experimental and theoretical investigations provided insights into the HER mechanisms of LaCeOx @NGr/Ru1 based on three indispensable steps: water adsorption and dissociation on Ov-rich LaCeOx, diffusion of generated H* species towards Ce3+-N-Ru1 bridges, and hydrogen evolution on Ru1 sites.
期刊介绍：
Applied Catalysis B: Environment and Energy (formerly Applied Catalysis B: Environmental) is a journal that focuses on the transition towards cleaner and more sustainable energy sources. The journal's publications cover a wide range of topics, including:
1.Catalytic elimination of environmental pollutants such as nitrogen oxides, carbon monoxide, sulfur compounds, chlorinated and other organic compounds, and soot emitted from stationary or mobile sources.
2.Basic understanding of catalysts used in environmental pollution abatement, particularly in industrial processes.
3.All aspects of preparation, characterization, activation, deactivation, and regeneration of novel and commercially applicable environmental catalysts.
4.New catalytic routes and processes for the production of clean energy, such as hydrogen generation via catalytic fuel processing, and new catalysts and electrocatalysts for fuel cells.
5.Catalytic reactions that convert wastes into useful products.
6.Clean manufacturing techniques that replace toxic chemicals with environmentally friendly catalysts.
7.Scientific aspects of photocatalytic processes and a basic understanding of photocatalysts as applied to environmental problems.
8.New catalytic combustion technologies and catalysts.
9.New catalytic non-enzymatic transformations of biomass components.
The journal is abstracted and indexed in API Abstracts, Research Alert, Chemical Abstracts, Web of Science, Theoretical Chemical Engineering Abstracts, Engineering, Technology & Applied Sciences, and others.
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