Understanding Boosted Selective CO2-to-CO Photoreduction with Pure Water Vapor over Hierarchical Biomass-Derived Carbon Matrix

Research output: Journal Publications and ReviewsRGC 21 - Publication in refereed journalpeer-review

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Author(s)

  • Zhifeng Jiang
  • Zhiquan Zhang
  • Min Zhou
  • Daobin Liu
  • Danjun Mao
  • Qun Zhang
  • Wei Zhang
  • Huaming Li
  • Li Song
  • Taicheng An
  • Po Keung Wong

Detail(s)

Original languageEnglish
Article number2301785
Journal / PublicationAdvanced Functional Materials
Volume33
Issue number29
Online published18 Apr 2023
Publication statusPublished - 18 Jul 2023

Abstract

Solar-driven CO2 reduction reaction (CO2RR) with water into carbon-neutral fuels is of great significance but remains challenging due to thermodynamic stability and kinetic inertness of CO2. Biomass-derived nitrogen-doped carbon (N-Cb) have been considered as promising earth-abundant photocatalysts for CO2RR, although their activities are not ideal and the reaction mechanism is still unclear. Herein, an efficient catalyst is developed for CO2-to-CO conversion realized on diverse N-Cb materials with hierarchical pore structures. It is demonstrated that the CO2-to-CO conversion preferentially takes place on positively charged carbon atoms next to pyridinic-N using two representatives treated pollens with the largest difference in pyridinic-N density and N content as model photocatalysts. Systematic experimental results indicate that surface local electric field originating from charge separation can be boosted by hierarchical pore structures, doped N, as well as pyridinic-N. Mechanistic studies reveal that positively charged carbon atoms next to pyridinic-N serve as active sites for CO2RR, reduce the energy barrier on the formation of CO*, and facilitate the CO2RR performance. All these benefits cooperatively contribute to treated chrysanthemum pollen catalyst exhibiting excellent CO formation rate of 203.2 µmol h−1 g−1 with 97.2% selectivity in pure water vapor. These results provide a new perspective into CO2RR on N-Cb, which shall guide the design of nature-based photocatalysts for high-performance solar-fuel generation. © 2023 Wiley-VCH GmbH.

Research Area(s)

  • carbon-based materials, metal-free catalysts, nitrogen doping, photocatalytic CO 2 reduction

Citation Format(s)

Understanding Boosted Selective CO2-to-CO Photoreduction with Pure Water Vapor over Hierarchical Biomass-Derived Carbon Matrix. / Jiang, Zhifeng; Zhang, Zhiquan; Liang, Jianli et al.
In: Advanced Functional Materials, Vol. 33, No. 29, 2301785, 18.07.2023.

Research output: Journal Publications and ReviewsRGC 21 - Publication in refereed journalpeer-review