Zhang Hongwen, Zhang Pu, Zhao Jiwu, Liu Yuan, Huang Yi, Huang Haowei, Yang Chen, Zhao Yibo, Wu Kaifeng, Fu Xianliang, Jin Shengye, Hou Yidong, Ding Zhengxin, Yuan Rusheng, Roeffaers Maarten B J, Zhong Shuncong, Long Jinlin
State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350116, P. R. China.
Laboratory of Optics, Terahertz and Nondestructive Testing, College of Mechanical Engineering and Automation, Fuzhou University, Fuzhou, 350116, P. R. China.
Angew Chem Int Ed Engl. 2021 Jul 12;60(29):16009-16018. doi: 10.1002/anie.202102983. Epub 2021 Jun 9.
Single-atom metal-insulator-semiconductor (SMIS) heterojunctions based on Sn-doped Fe O nanorods (SF NRs) were designed by combining atomic deposition of an Al O overlayer with chemical grafting of a RuO hole-collector for efficient CO -to-syngas conversion. The RuO -Al O -SF photoanode with a 3.0 nm thick Al O overlayer gave a >5-fold-enhanced IPCE value of 52.0 % under 370 nm light irradiation at 1.2 V vs. Ag/AgCl, compared to the bare SF NRs. The dielectric field mediated the charge dynamics at the Al O /SF NRs interface. Accumulation of long-lived holes on the surface of the SF NRs photoabsorber aids fast tunneling transfer of hot holes to single-atom RuO species, accelerating the O -evolving reaction kinetics. The maximal CO-evolution rate of 265.3 mmol g h was achieved by integration of double SIMS-3 photoanodes with a single-atom Ni-doped graphene CO -reduction-catalyst cathode; an overall quantum efficiency of 5.7 % was recorded under 450 nm light irradiation.
通过将AlO覆盖层的原子沉积与RuO空穴收集器的化学接枝相结合，设计了基于Sn掺杂的FeO纳米棒（SF NRs）的单原子金属-绝缘体-半导体（SMIS）异质结，用于高效的CO转化为合成气。与裸露的SF NRs相比，具有3.0 nm厚AlO覆盖层的RuO-AlO-SF光阳极在1.2 V vs. Ag/AgCl的条件下，在370 nm光照射下的IPCE值提高了5倍以上，达到52.0%。介电场介导了AlO/SF NRs界面处的电荷动力学。SF NRs光吸收体表面长寿命空穴的积累有助于热空穴快速隧穿转移到单原子RuO物种，加速析氧反应动力学。通过将双SIMS-3光阳极与单原子Ni掺杂石墨烯CO还原催化剂阴极集成，实现了265.3 mmol g h的最大CO析出速率；在450 nm光照射下，记录的总量子效率为5.7%。
