Yu Nie , Yanfang Li , Chao An , Xin Tan , Zhuofeng Hu , Jinhua Ye , Tao Yu
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引用次数: 0
摘要
二氧化碳还原生成乙烯的过程缓慢，因为存在排斥性偶极-偶极相互作用和连续的 12 个质子耦合电子转移步骤。非晶态结构的光催化剂晶界少，不饱和位点多，从动力学和热力学的角度提高了反应效率，但目前尚未应用于 PCR 制备 C2 产物。本文制备了由少数晶体 CuCo2S4 组成的非晶态 CuxCoSy，实现了出色的 C2H4 电子选择性（94.9%）。不饱和 Co 和 S 在提高 C2H4 生成效率方面发挥了关键作用。通过缩短 Co-S 键的距离实现了 C-C 耦合，而⁎CO-⁎CO 耦合势垒则通过在不饱和 S 上积累更多的电子而降低。水吸附在与 S 相邻的 Co 上，为⁎CO 形成⁎CH2=C 提供了质子。这项工作为利用非晶光催化剂扩大 C2H4 光催化进化的效率铺平了新的道路。
Promoted selectivity of photocatalytic CO2 reduction to C2H4 via hybrid CuxCoSy possessing dual unsaturated sites
Ethylene production by CO2 reduction is sluggish because the repulsive dipole-dipole interaction and 12 proton-coupled electron-transfer steps consecutively. Amorphous structured photocatalysts possess few grain boundaries and abundant unsaturated sites, accelerating the reaction efficiency from the angle of dynamics and thermodynamics, which still not yet be used in PCR to C2 products currently. Herein, an amorphous CuxCoSy composed of the minority crystalline CuCo2S4 is fabricated to realize an excellent C2H4 selectivity in terms of Relectron (94.9%). Unsaturated Co and S play the key roles in the improved efficiency of C2H4 generation. C-C coupling is achieved via shortening Co-S bonds distance, and *CO-*CO coupling barrier is decreased by more electrons accumulated on unsaturated S. Water is adsorbed on Co adjacent to S and provide protons for *COCO to form *CH2 = C. This work paves a new way for broadening the efficient of C2H4 photocatalytic evolution using amorphous photocatalyst.
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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