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Graphdiyne: A New Photocatalytic CO_2 Reduction Cocatalyst

机译：Graphdiyne：一种新型的光催化CO_2还原助催化剂

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摘要

Exploring new and efficient cocatalysts to boost photocatalytic CO2 reduction is of critical importance for solar-to-fuel conversion. As an emerging carbon allotrope, graphdiyne (GDY) features 2D characteristics and unique carbon-carbon bonds. Herein, a novel GDY cocatalyst coupled TiO2 nanofibers for boosted photocatalytic CO2 reduction, synthesized by an electrostatic self-assembly approach is reported. First-principle calculation and in situ X-ray photoelectron spectroscopy measurement reveal that the delocalized electrons in GDY can hybrid with the empty orbitals in TiO2 within the TiO2/GDY network, leading to the formation of an internal electric field at the interfaces, pointing from GDY to TiO2. The theoretical simulation further implies strong chemisorption and deformation of CO2 molecules upon GDY, which can be verified by in situ diffuse reflectance infrared Fourier transform spectroscopy. These effects, in combination with the photothermal effect of GDY, result in enhanced charge separation and directed electron transfer, enhanced CO2 adsorption and activation as well as accelerated catalytic reactions over the TiO2/GDY heterostructure, thereby resulting in significantly improved CO2 photoreduction efficiency and meanwhile with remarkable selectivity. This work demonstrates that GYD can function as a highly effective cocatalyst for solar energy harvesting and may be used in other catalysis processes.
机译：探索新型高效的助催化剂以促进光催化二氧化碳的还原对于太阳能转化为燃料至关重要。作为新兴的碳同素异形体，石墨二炔（GDY）具有2D特性和独特的碳碳键。本文中，报道了通过静电自组装方法合成的新型GDY助催化剂偶联的TiO 2纳米纤维，用于增强光催化CO 2还原。第一性原理计算和原位X射线光电子能谱测量表明，GDY中的离域电子可以与TiO2 / GDY网络中TiO2中的空轨道杂化，从而导致在界面处形成内部电场，从GDY为TiO2。理论模拟进一步暗示了CO2分子在GDY上的强烈化学吸附和变形，这可以通过原位漫反射红外傅里叶变换光谱法进行验证。这些效应与GDY的光热效应相结合，可增强电荷分离和定向电子转移，增强TiO2 / GDY异质结构上的CO2吸附和活化以及加速的催化反应，从而显着提高CO2的光还原效率，同时具有卓越的选择性。这项工作表明，GYD可以充当太阳能收集的高效助催化剂，并可以用于其他催化过程。

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