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The Hole-Tunneling Heterojunction of Hematite-Based Photoanodes Accelerates Photosynthetic Reaction

  • Zhang, Hongwen; 141588;
  • Zhang, Pu;
  • Zhao, Jiwu;
  • Liu, Yuan;
  • Huang, Yi;
  • Huang, Haowei; 113034;
  • Yang, Chen;
  • Zhao, Yibo;
  • Wu, Kaifeng;
  • Fu, Xianliang;
  • Jin, Shengye;
  • Hou, Yidong;
  • Ding, Zhengxin;
  • Yuan, Rusheng;
  • Roeffaers, Maarten BJ; 46986;
  • Zhong, Shuncong;
  • Long, Jinlin;
Publication Date
Jun 09, 2021
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Single-atom metal-insulator-semiconductor (SMIS) heterojunctions based on Sn-doped Fe2 O3 nanorods (SF NRs) were designed by combining atomic deposition of an Al2 O3 overlayer with chemical grafting of a RuOx hole-collector for efficient CO2 -to-syngas conversion. The RuOx -Al2 O3 -SF photoanode with a 3.0 nm thick Al2 O3 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 Al2 O3 /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 RuOx species, accelerating the O2 -evolving reaction kinetics. The maximal CO-evolution rate of 265.3 mmol g-1 h-1 was achieved by integration of double SIMS-3 photoanodes with a single-atom Ni-doped graphene CO2 -reduction-catalyst cathode; an overall quantum efficiency of 5.7 % was recorded under 450 nm light irradiation. / status: published

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