材料科学
光催化
异质结
X射线光电子能谱
制氢
人工光合作用
锐钛矿
载流子
分解水
超快激光光谱学
光化学
氢
纳米技术
光谱学
光电子学
化学工程
催化作用
化学
物理
有机化学
量子力学
工程类
作者
Xiaowen Ruan,Chengxiang Huang,Hui Cheng,Zhiquan Zhang,Yi Cui,Zhi-Yun Li,Tengfeng Xie,Kaikai Ba,Haiyan Zhang,Lei Zhang,Xiao Zhao,Jing Leng,Shengye Jin,Wei Zhang,Weitao Zheng,Sai Kishore Ravi,Zhifeng Jiang,Xiaoqiang Cui,Jiaguo Yu
标识
DOI:10.1002/adma.202209141
摘要
Designing heterojunction photocatalysts imitating natural photosynthetic systems has been a promising approach for photocatalytic hydrogen generation. However, in the traditional Z-Scheme artificial photosynthetic systems, the poor charge separation, and rapid recombination of photogenerated carriers remain a huge bottleneck. To rationally design S-Scheme (i.e., Step scheme) heterojunctions by avoiding the futile charge transport routes is therefore seen as an attractive approach to achieving high hydrogen evolution rates. Herein, a twin S-scheme heterojunction is proposed involving graphitic C3 N4 nanosheets self-assembled with hydrogen-doped rutile TiO2 nanorods and anatase TiO2 nanoparticles. This catalyst shows an excellent photocatalytic hydrogen evolution rate of 62.37 mmol g-1 h-1 and high apparent quantum efficiency of 45.9% at 365 nm. The significant enhancement of photocatalytic performance is attributed to the efficient charge separation and transfer induced by the unique twin S-scheme structure. The charge transfer route in the twin S-scheme is confirmed by in situ X-ray photoelectron spectroscopy (XPS) and electron spin resonance (ESR) spin-trapping tests. Femtosecond transient absorption (fs-TA) spectroscopy, transient-state surface photovoltage (TPV), and other ex situ characterizations further corroborate the efficient charge transport across the catalyst interface. This work offers a new perspective on constructing artificial photosynthetic systems with S-scheme heterojunctions to enhance photocatalytic performance.
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