光催化
Boosting(机器学习)
氢
电荷(物理)
分离(统计)
材料科学
化学工程
纳米技术
化学
催化作用
工程类
物理
计算机科学
人工智能
有机化学
量子力学
机器学习
作者
Jingwen Pan,Dongbo Wang,Bingke Zhang,Chenchen Zhao,Donghao Liu,Sihang Liu,Zhi Zeng,Tianyuan Chen,Gang Liu,Shujie Jiao,Zhikun Xu,Tongling Liu,Taifeng Liu,Xuan Fang,Liancheng Zhao,Jinzhong Wang
标识
DOI:10.1016/j.cej.2024.150536
摘要
The synergistic implementation of atomic-level charge separation strategies for bulk–surfaces is a meaningful study that fundamentally addresses the shortcomings of single materials. Here, we report for the first time the atomic-level engineering of atomic doping in combination with surface ion grafting, which can be coordinated to significantly facilitate photocatalytic H2 evolution. More impressively, the study systematically investigated the atomic doping effects of Fe, Co, Ni and Cu atoms, and analyzed the conditions for optimal doping with experimental and theoretical calculations. Electrons from the Cu were transferred to Zn0.67Cd0.33S or adsorbed H atoms on its surface, effectively enhancing the surface charge density and electron transport capacity. The X-ray absorption spectroscopy (XAS) results verified the precise coordination environments of the doped Cu atoms, as well as confirmed the solid grafting of Ni ions on the catalyst surface. Furthermore, the hydrogen production rate of 1.2 % Cu–Zn0.67Cd0.33S–0.5 wt% Ni reached 38.17 mmol/g/h, corresponding to an apparent quantum efficiency of 35.5 %, which is 82.8 times higher than that of pure ZCS. Besides, the H2 production rate can reached 118.73 mmol/g/h without cooling. Meanwhile, the synergistic strategy of manipulating the bulk and surface photo-charges of Zn0.67Cd0.33S also effectively enhances the photothermal effect and further improves its photocatalytic performance. This work provides different inspirations for bottom-up design of efficient photocatalysts to achieve synergistic facilitation strategies.
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