首页|Reconcile the contradictory wettability requirements for the reduction and oxidation half-reactions in overall CO2 photoreduction via alternately hydrophobic surfaces

Reconcile the contradictory wettability requirements for the reduction and oxidation half-reactions in overall CO2 photoreduction via alternately hydrophobic surfaces

扫码查看
原文链接
  • NETL
  • NSTL
  • 万方数据
The overall photocatalytic CO2 reduction reaction(OPCRR)that can directly convert CO2 and H2O into fuels represents a promising renewable energy conversion technology.As a typical redox reaction,the OPCRR involves two half-reactions:the CO2 reduction half-reaction(CRHR)and the water oxidation half-reaction(WOHR).Generally,both half-reactions can be promoted by adjusting the wettability of cat-alysts.However,there is a contradiction in wettability requirements for the two half-reactions.Specifically,CRHR prefers a hydrophobic surface that can accumulate more CO2 molecules on the active sites,ensuring the appropriate ratio of gas-phase(CO2)to liquid-phase(H2O)reactants.Conversely,the WOHR prefers a hydrophilic surface that can promote the departure of the gaseous product(O2)from the catalyst surface,preventing isolation between active sites and the reactant(H2O).Here,we successfully reconciled the contradictory wettability requirements for the CRHR and WOHR by creating an alternately hydrophobic catalyst.This was achieved through a selectively hydrophobic modification method and a charge-transfer-control strategy.Consequently,the collaboratively promoted CRHR and WOHR led to a significantly enhanced OPCRR with a solar-to-fuel conversion efficiency of 0.186％.Notably,in ethanol production,the catalyst exhibited a 10.64-fold increase in generation rate(271.44 pmol g-1 h-1)and a 4-fold increase in selectivity(55.77％)compared to the benchmark catalyst.This innovative approach holds great potential for application in universal overall reactions involving gas participation.

HydrophobicHydrophilicGas transportOverall CO2 photoreductionZ-scheme

Hailing Huo、Ting Hu、Chengxi Huang、Fang Wu、Tongyu Wang、Xuan Liu、Liang Zhang、Qiang Ju、Zhiqing Zhong、Hongbin Xing、Erjun Kan、Ang Li

展开 >

MIIT Key Laboratory of Semiconductor Microstructure and Quantum Sensing,Nanjing University of Science and Technology,Nanjing 210094,Jiangsu,China

College of Information Science and Technology,Nanjing Forestry University,Nanjing 210037,Jiangsu,China

National Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNational Outstanding Youth Science Fund Project of National Natural Science Foundation of ChinaFunding of NJUSTPostgraduate Research &Practice Innovation Program of Jiangsu Province

223782042200812151790492T2125004TSXK2022D002KYCX23_0454

2024

10.1016/j.jechem.2024.02.010

能源化学
中国科学院大连化学物理研究所 中国科学院成都有机化学研究所

能源化学

CSTPCDEI
影响因子：0.654
ISSN：2095-4956
年,卷(期)：2024.93(6)
  • 51