Advanced Science (Oct 2017)

Photothermal Catalyst Engineering: Hydrogenation of Gaseous CO2 with High Activity and Tailored Selectivity

  • Jia Jia,
  • Hong Wang,
  • Zhuole Lu,
  • Paul G. O'Brien,
  • Mireille Ghoussoub,
  • Paul Duchesne,
  • Ziqi Zheng,
  • Peicheng Li,
  • Qiao Qiao,
  • Lu Wang,
  • Alan Gu,
  • Feysal M. Ali,
  • Yuchan Dong,
  • Qiang Wang,
  • Kulbir Kaur Ghuman,
  • Thomas Wood,
  • Chenxi Qian,
  • Yue Shao,
  • Chenyue Qiu,
  • Miaomiao Ye,
  • Yimei Zhu,
  • Zheng‐Hong Lu,
  • Peng Zhang,
  • Amr S. Helmy,
  • Chandra Veer Singh,
  • Nazir P. Kherani,
  • Doug D. Perovic,
  • Geoffrey A. Ozin

DOI
https://doi.org/10.1002/advs.201700252
Journal volume & issue
Vol. 4, no. 10
pp. n/a – n/a

Abstract

Read online

Abstract This study has designed and implemented a library of hetero‐nanostructured catalysts, denoted as Pd@Nb2O5, comprised of size‐controlled Pd nanocrystals interfaced with Nb2O5 nanorods. This study also demonstrates that the catalytic activity and selectivity of CO2 reduction to CO and CH4 products can be systematically tailored by varying the size of the Pd nanocrystals supported on the Nb2O5 nanorods. Using large Pd nanocrystals, this study achieves CO and CH4 production rates as high as 0.75 and 0.11 mol h−1 gPd−1, respectively. By contrast, using small Pd nanocrystals, a CO production rate surpassing 18.8 mol h−1 gPd−1 is observed with 99.5% CO selectivity. These performance metrics establish a new milestone in the champion league of catalytic nanomaterials that can enable solar‐powered gas‐phase heterogeneous CO2 reduction. The remarkable control over the catalytic performance of Pd@Nb2O5 is demonstrated to stem from a combination of photothermal, electronic and size effects, which is rationally tunable through nanochemistry.

Keywords