Kangwang Wang, Mingjie Wu, Peifeng Yu, Hector F. Garces, Ying Liang, Longfu Li, Lingyong Zeng, Kuan Li, Chao Zhang, Kai Yan, Huixia Luo
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引用次数: 0
摘要
尽管研究工作仍在进行,但如何合理设计用于选择性光催化 CO$_2$ 转化为有价值产品的非复杂拓扑半金属表面态仍然充满挑战。在此,我们通过实验工作和理论计算的结合,介绍了 1T-OsCoTe$_2$ 的合成,用于 CO$_2$ 的光催化升级为碳烷烃 C$_3$H$_8$。实验研究表明,C$_3$H$_8$的电子选择性高达 71.2%,在 380 纳米波长下的内部量子效率为 54.6%。原位 X 射线光电子能谱和 X 射线吸收精细结构能谱表明,与 Te 原子配位的 Co 原子和 Os 原子能够实现高效的 Os-Te-Co 电子转移,从而激活*CH$_3$、*CHOCO 和*CH$_2$OCOCO 的生成。密度泛函理论计算进一步证实了 Os-Te-Co 电子桥接对 CO$_2$ 转化动力学的改善作用。据我们所知,这是第一份关于 Osatoms 在加速拓扑半金属 1T-OsCoTe$_2$ 的光催化 CO$_2$ 转化活性中的作用的报告。
Non-trivial Topological Surface States Regulation of 1T-OsCoTe$_2$ Enables Selective C-C Coupling for Highly Efficient Photochemical CO$_2$ Reduction Toward C$_{2+}$ hydrocarbons
Despite ongoing research, the rational design of nontrivial topological
semimetal surface states for the selective photocatalytic CO$_2$ conversion
into valuable products remains full of challenges. Herein, we present the
synthesis of 1T-OsCoTe$_2$ for the photoreduction upgrading of CO$_2$ to
tricarbon alkane C$_3$H$_8$,by the integration of experimental work and theory
calculation. Experimental studies suggested a high electron based selectivity
of 71.2% for C$_3$H$_8$ and an internal quantum efficiency of 54.6% at 380 nm.
In-situ X-ray photoelectron spectroscopy and X-ray absorption fine structure
spectroscopy demonstrated that Co and Os atoms coordinated with Te atoms enable
an efficient Os-Te-Co electron transfer to activate the generation of
*CH$_3$,*CHOCO and *CH$_2$OCOCO. Density functional theory calculations further
confirmed Os-Te-Co electron bridging on the improved CO$_2$ conversion
kinetics. To our knowledge, this is the first report suggesting the role of Os
atoms in accelerating the photocatalytic CO$_2$ conversion activity of the
topological semimetal 1T-OsCoTe$_2$.