Photothermal Synergistic Catalysis over Defective Zn 3 In 2 S 6 for CO 2 Fixation

作者：Weilong Zhang, Zhuo Li, Xue-fang Yu, Kaisheng Zhang, Senmiao Liu, Yujie Du, Qi Guo, Lixue Zhang, Xin Ding, Hua Tang, Yanhua Peng, Xiaolong Yang · 发表于：Inorganic Chemistry · 年份：2024 · DOI：10.1021/acs.inorgchem.3c03520 · 被引用次数：49 · 研究领域：Carbon dioxide utilization in catalysis、Advanced Photocatalysis Techniques、CO2 Reduction Techniques and Catalysts

Carbon dioxide (CO 2 ) cycloaddition not only produces highly valued cyclic carbonate but also utilizes CO 2 as C1 resources with 100% atomic efficiency. However, traditional catalytic routes still suffer from inferior catalytic efficiency and harsh reaction conditions. Developing multienergy-field catalytic technology with expected efficiency offers great opportunity for satisfied yield under mild conditions. Herein, Zn 3 In 2 S 6 with sulfur vacancies (S v ) was fabricated with the assistance of cetyltrimethylammonium bromide (CTAB), which is further employed for photothermally driven CO 2 cycloaddition first. Photoluminescence spectroscopy and photoelectrochemical characterization demonstrated its superior separation kinetics of photoinduced carriers induced by defect engineering. The temperature-programmed desorption (TPD) technique indicated its excellent Lewis acidity–basicity characters. Due to the combination of above merits from photocatalysis and thermal catalysis, defective Zn 3 In 2 S 6 -S v achieved a yield as high as 73.2% for cyclic carbonate at 80 °C under blue LED illumination within 2 h (apparent quantum yield of 0.468% under illumination of 380 nm monochromatic light at 36 mW·cm –2 ), which is 2.9, 2.0, and 6.9 times higher than that in dark conditions and those of pristine Zn 3 In 2 S 6 and industrial representative tetrabutylammonium bromide (TBAB) thermal-catalysis process under the same conditions, respectively. The synergistic reaction path of photocat...