Jiang Wenbin, Zhu Hui, Yang Jing, Low Beverly Qian Ling, Wu Wen-Ya, Chen Mingxi, Ma Jun, Long Ran, Low Jingxiang, Zhu Houjuan, Heng Jerry Zhi Xiong, Tang Karen Yuanting, Chai Casandra Hui Teng, Lin Ming, Zhu Qiang, Zhang Yong-Wei, Chi Dongzhi, Li Zibiao, Loh Xian Jun, Xiong Yujie, Ye Enyi
Institute of Materials Research and Engineering (IMRE), Agency for Science, Technology and Research (A*STAR), 2 Fusionopolis Way, Innovis #08-03, Singapore, 138634, Republic of Singapore.
School of Electrical and Electronic Engineering, Nanyang Technological University, 50 Nanyang Avenue, Singapore, 639798, Republic of Singapore.
Adv Sci (Weinh). 2023 Oct;10(28):e2303448. doi: 10.1002/advs.202303448. Epub 2023 Aug 6.
Piezo-assisted photocatalysis (namely, piezo-photocatalysis), which utilizes mechanical energy to modulate spatial and energy distribution of photogenerated charge carriers, presents a promising strategy for molecule activation and reactive oxygen species (ROS) generation toward applications such as environmental remediation. However, similarly to photocatalysis, piezo-photocatalysis also suffers from inferior charge separation and utilization efficiency. Herein, a Z-scheme heterojunction composed of single Ag atoms-anchored polymeric carbon nitride (Ag-PCN) and SnO is developed for efficient charge carrier transfer/separation both within the catalyst and between the catalyst and surface oxygen molecules (O ). As revealed by charge dynamics analysis and theoretical simulations, the synergy between the single Ag atoms and the Z-scheme heterojunction initiates a cascade electron transfer from SnO to Ag-PCN and then to O adsorbed on Ag. With ultrasound irradiation, the polarization field generated within the piezoelectric hybrid further accelerates charge transfer and regulates the O activation pathway. As a result, the Ag-PCN/SnO catalyst efficiently activates O into ·O , ·OH, and H O under co-excitation of visible light and ultrasound, which are consequently utilized to trigger aerobic degradation of refractory antibiotic pollutants. This work provides a promising strategy to maneuver charge transfer dynamics for efficient piezo-photocatalysis by integrating single-atom catalysts (SACs) with Z-scheme heterojunction.
压电辅助光催化（即压电光催化）利用机械能来调节光生电荷载流子的空间和能量分布，为分子活化和活性氧（ROS）生成提供了一种有前景的策略，可应用于环境修复等领域。然而，与光催化类似，压电光催化也存在电荷分离和利用效率低下的问题。在此，开发了一种由单原子银锚定的聚合氮化碳（Ag-PCN）和SnO组成的Z型异质结，用于在催化剂内部以及催化剂与表面氧分子（O）之间实现高效的电荷载流子转移/分离。电荷动力学分析和理论模拟表明，单原子银与Z型异质结之间的协同作用引发了从SnO到Ag-PCN再到吸附在银上的O的级联电子转移。在超声辐照下，压电复合材料内部产生的极化场进一步加速电荷转移并调节O的活化途径。结果，Ag-PCN/SnO催化剂在可见光和超声的共同激发下有效地将O活化为·O 、·OH和H O，进而用于引发难降解抗生素污染物的好氧降解。这项工作通过将单原子催化剂（SACs）与Z型异质结相结合，为操纵电荷转移动力学以实现高效压电光催化提供了一种有前景的策略。
