Zhou Xiyuan, Wang Kaiwen, Wang Yang, Cao Yongyong, Wang Jiaxing, Hu Hanwen, Yang Guo, Hou Jixiang, Ma Peijie, Gao Chunlang, Ban Chaogang, Duan Youyu, Wei Zhen, Zhang Xu, Wang Cong, Zheng Kun
Beijing Key Laboratory of Microstructure and Properties of Solids, College of Materials Science and Engineering, Beijing University of Technology, Beijing 100124, China.
School of Optoelectronic Engineering & CQUPT-BUL Innovation Institute, Chongqing University of Posts and Telecommunications, Chongqing 400065, China.
Langmuir. 2024 May 28;40(21):11251-11262. doi: 10.1021/acs.langmuir.4c01014. Epub 2024 May 15.
Artificial photosynthesis for high-value hydrogen peroxide (HO) through a two-electron reduction reaction is a green and sustainable strategy. However, the development of highly active HO photocatalysts is impeded by severe carrier recombination, ineffective active sites, and low surface reaction efficiency. We developed a dual optimization strategy to load dense Ni nanoparticles onto ultrathin porous graphitic carbon nitride (Ni-UPGCN). In the absence and presence of sacrificial agents, Ni-UPGCN achieved HO production rates of 169 and 4116 μmol g h with AQY (apparent quantum efficiency) at 420 nm of 3.14% and 17.71%. Forming a Schottky junction, the surface-modified Ni nanoparticles broaden the light absorption boundary and facilitate charge separation, which act as active sites, promoting O adsorption and reducing the formation energy of *OOH (reaction intermediate). This results in a substantial improvement in both HO generation activity and selectivity. The Schottky junction of dual modulation strategy provides novel insights into the advancement of highly effective photocatalytic agents for the photosynthesis of HO.
通过双电子还原反应人工合成高价值过氧化氢(HO)是一种绿色且可持续的策略。然而,严重的载流子复合、无效的活性位点和较低的表面反应效率阻碍了高活性HO光催化剂的发展。我们开发了一种双重优化策略,将致密的镍纳米颗粒负载到超薄多孔石墨相氮化碳(Ni-UPGCN)上。在不存在和存在牺牲剂的情况下,Ni-UPGCN的HO产率分别为169和4116 μmol g h,在420 nm处的表观量子效率(AQY)分别为3.14%和17.71%。表面改性的镍纳米颗粒形成肖特基结,拓宽了光吸收边界并促进电荷分离,这些镍纳米颗粒作为活性位点,促进O吸附并降低*OOH(反应中间体)的形成能。这导致HO生成活性和选择性都有显著提高。双调制策略的肖特基结为开发用于HO光合作用的高效光催化剂提供了新的见解。