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Distance Synergy of MoS2-Confined Rhodium Atoms for Highly Efficient Hydrogen Evolution |
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| Authors: | Xiangyu Meng Prof Dr Chao Ma Luozhen Jiang Prof Dr Rui Si Prof Dr Xianguang Meng Dr Yunchuan Tu Prof Dr Liang Yu Prof Dr Xinhe Bao Prof Dr Dehui Deng |
| Institution: | 1. State Key Laboratory of Catalysis,iChEM, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Zhongshan Road 457, Dalian, 116023 China
University of Chinese Academy of Sciences, Beijing, 100039 China State Key Laboratory of Physical Chemistry of Solid Surfaces,iChEM, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005 China;2. College of Materials Science and Engineering, Hunan University, Changsha, 410082 China;3. University of Chinese Academy of Sciences, Beijing, 100039 China Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai, 201204 China;4. Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai, 201204 China;5. State Key Laboratory of Catalysis,iChEM, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Zhongshan Road 457, Dalian, 116023 China;6. State Key Laboratory of Catalysis,iChEM, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Zhongshan Road 457, Dalian, 116023 China University of Chinese Academy of Sciences, Beijing, 100039 China |
| Abstract: | Perturbing the electronic structure of the MoS2 basal plane by confining heteroatoms offers the opportunity to trigger in-plane activity for the hydrogen evolution reaction (HER). The key challenge consists of inducing the optimum HER activity by controlling the type and distribution of confined atoms. A distance synergy of MoS2-confined single-atom rhodium is presented, leading to an ultra-high HER activity at the in-plane S sites adjacent to the rhodium. By optimizing the distance between the confined Rh atoms, an ultra-low overpotential of 67 mV is achieved at a current density of 10 mA cm−2 in acidic solution. Experiments and first-principles calculations demonstrate a unique distance synergy between the confined rhodium atoms in tuning the reactivity of neighboring in-plane S atoms, which presents a volcanic trend with the inter-rhodium distance. This study provides a new strategy to tailor the activity of MoS2 surface via modulating the distance between confined single atoms. |
| Keywords: | confined heteroatoms distance synergy electrocatalysis hydrogen evolution reaction MoS2 |