Zhang Fu-Guang, Chen Yan, Ma Chi, Tang Ji-Ping, Wang Zi-Yi, Zhao Zong-Yan, Bao Liang, Yuan Yong-Jun
College of Materials and Environmental Engineering, Hangzhou Dianzi University, Hangzhou 310018, People's Republic of China.
Faculty of Materials Science and Engineering, Kunming University of Science and Technology, Kunming 650093, People's Republic of China.
Inorg Chem. 2024 Jul 22;63(29):13766-13774. doi: 10.1021/acs.inorgchem.4c02147. Epub 2024 Jul 5.
Solar photocatalytic H production from lignocellulosic biomass has attracted great interest, but it suffers from low photocatalytic efficiency owing to the absence of highly efficient photocatalysts. Herein, we designed and constructed ultrathin MoS-modified porous TiO microspheres (MT) with abundant interface Ti-S bonds as photocatalysts for photocatalytic H generation from lignocellulosic biomass. Owing to the accelerated charge transfer related to Ti-S bonds, as well as the abundant active sites for both H and OH generation, respectively, related to the high exposed edge of MoS and the large specific surface area of TiO, MT photocatalysts demonstrate good performance in the photocatalytic conversion of α-cellulose and lignocellulosic biomass to H. The highest H generation rate of 849 μmol·g·h and apparent quantum yield of 4.45% at 380 nm was achieved in α-cellulose aqueous solution for the optimized MT photocatalyst. More importantly, lignocellulosic biomass of corncob, rice hull, bamboo, polar wood chip, and wheat straw were successfully converted to H over MT photocatalysts with H generation rate of 10, 19, 36, 29, and 8 μmol·g·h, respectively. This work provides a guiding design approach to develop highly active photocatalysts via interface engineering for solar H production from lignocellulosic biomass.
利用木质纤维素生物质通过太阳能光催化产氢引起了广泛关注,但由于缺乏高效光催化剂,其光催化效率较低。在此,我们设计并构建了具有丰富界面Ti-S键的超薄MoS修饰多孔TiO微球(MT)作为光催化剂,用于从木质纤维素生物质中光催化产氢。由于与Ti-S键相关的电荷转移加速,以及分别与MoS的高暴露边缘和TiO的大比表面积相关的用于生成H和OH的丰富活性位点,MT光催化剂在将α-纤维素和木质纤维素生物质光催化转化为H方面表现出良好性能。在α-纤维素水溶液中,优化后的MT光催化剂实现了最高产氢速率849 μmol·g·h和380 nm处4.45%的表观量子产率。更重要的是,玉米芯、稻壳、竹子、极地木屑和小麦秸秆等木质纤维素生物质在MT光催化剂上成功转化为H,产氢速率分别为10、19、36、29和8 μmol·g·h。这项工作提供了一种指导设计方法,通过界面工程开发用于从木质纤维素生物质中太阳能产氢的高活性光催化剂。