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一步磷化法制备具有多通道电荷分离功能的梯度磷掺杂CdS/CoP杂化纳米棒用于光催化水还原

One-step phosphorization preparation of gradient-P-doped CdS/CoP hybrid nanorods having multiple channel charge separation for photocatalytic reduction of water.

作者信息

Guo Changfa, Li Lei, Chen Fang, Ning Jiqiang, Zhong Yijun, Hu Yong

机构信息

Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, Department of Chemistry, Zhejiang Normal University, Jinhua 321004, China.

Hangzhou Institute of Advanced Studies, Zhejiang Normal University, Hangzhou, Zhejiang 311231, China.

出版信息

J Colloid Interface Sci. 2021 Aug 15;596:431-441. doi: 10.1016/j.jcis.2021.03.170. Epub 2021 Mar 31.

DOI:10.1016/j.jcis.2021.03.170
PMID:33848747
Abstract

The separation and transfer of photogenerated charge carriers are the crucial process in photocatalysis, and the realization of multiple charge separation and transfer routes in a single catalyst structure is very promising to achieve high-efficiency catalytic performance. We herein report a simple strategy to synthesize CdS/CoP hybrid nanorods (HNRs) via a one-step phosphorization treatment of the CdS/Co(OH) precursors, in which the gradient-P-doped-CdS NRs and CoP cocatalyst can be synchronously obtained (denoted as gP-CdS/CoP HNRs). The gradient P doping gradually reduced the band gap of CdS as well as elevated Fermi level with doping concentration up, resulting in the formation of a built-in electric field in the CdS NRs. The built-in electric field points from the surface towards the interior of the CdS NRs, which facilities the separation of photogenerated charge carriers in CdS and the transfer of electrons to the CdS/CoP interface. The transferred electrons are then captured by the CoP cocatalysts, leading to further separation of the charge carriers. Owing to the coupling of gradient-P-doped CdS nanorods with the CoP cocatalysts, the optimized gP-CdS/CoP HNRs exhibit remarkably enhanced photocatalytic water reduction performance, with a H production rate of 22.95 mmol g h which is 28.7 and 3.2 times higher than that of pristine CdS and gP-CdS, respectively. This work demonstrates the synergetic effects of charge carrier separation in the coupled nanostructure of the gradient-P-doped CdS NRs with the CoP cocatalyst, which provides a new platform for developing heterostructures with multiple charge separation and transfer routes for photocatalysis.

摘要

光生电荷载流子的分离与转移是光催化过程中的关键步骤,在单一催化剂结构中实现多条电荷分离与转移途径对于实现高效催化性能非常有前景。在此,我们报道一种简单的策略,通过对CdS/Co(OH)前驱体进行一步磷化处理来合成CdS/CoP混合纳米棒(HNRs),其中可以同步获得梯度P掺杂的CdS纳米棒和CoP助催化剂(记为gP-CdS/CoP HNRs)。随着掺杂浓度的增加,梯度P掺杂逐渐减小了CdS的带隙并提高了费米能级,导致在CdS纳米棒中形成内建电场。内建电场从CdS纳米棒的表面指向内部,这有利于CdS中光生电荷载流子的分离以及电子向CdS/CoP界面的转移。转移的电子随后被CoP助催化剂捕获,导致电荷载流子的进一步分离。由于梯度P掺杂的CdS纳米棒与CoP助催化剂的耦合,优化后的gP-CdS/CoP HNRs表现出显著增强的光催化水还原性能,产氢速率为22.95 mmol g⁻¹ h⁻¹,分别比原始CdS和gP-CdS高28.7倍和3.2倍。这项工作证明了梯度P掺杂的CdS纳米棒与CoP助催化剂的耦合纳米结构中电荷载流子分离的协同效应,为开发具有多条电荷分离和转移途径的光催化异质结构提供了一个新平台。

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