氧化还原
异质结
材料科学
催化作用
电子转移
吸收光谱法
吸收(声学)
离子液体
光化学
光电子学
化学
物理
有机化学
光学
复合材料
冶金
作者
Ling Sun,Ziqing Zhang,Ji Bian,Fu‐Quan Bai,Hengwei Su,Zhijun Li,Jijia Xie,Rongping Xu,Jianhui Sun,Linlu Bai,Cailing Chen,Yu Han,Junwang Tang,Liqiang Jing
标识
DOI:10.1002/adma.202300064
摘要
Solar-driven CO2 reduction by water with a Z-scheme heterojunction affords an avenue to access energy storage and to alleviate greenhouse gas (GHG) emissions, yet the separation of charge carriers and the integrative regulation of water oxidation and CO2 activation sites remain challenging. Here, a BiVO4 /g-C3 N4 (BVO/CN) Z-scheme heterojunction as such a prototype is constructed by spatially separated dual sites with CoOx clusters and imidazolium ionic liquids (IL) toward CO2 photoreduction. The optimized CoOx -BVO/CN-IL delivers an ≈80-fold CO production rate without H2 evolution compared with urea-C3 N4 counterpart, together with nearly stoichiometric O2 gas produced. Experimental results and DFT calculations unveil the cascade Z-scheme charge transfer and subsequently the prominent redox co-catalysis by CoOx and IL for holes-H2 O oxidation and electrons-CO2 reduction, respectively. Moreover, in situ µs-transient absorption spectra clearly show the function of each cocatalyst and quantitatively reveal that the resulting CoOx -BVO/CN-IL reaches up to the electron transfer efficiency of 36.4% for CO2 reduction, far beyond those for BVO/CN (4.0%) and urea-CN (0.8%), underlining an exceptional synergy of dual reaction sites engineering. This work provides deep insights and guidelines for the rational design of highly efficient Z-scheme heterojunctions with precise redox catalytic sites toward solar fuel production.
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