Transient Solid-State Laser Activation of Indium for High-Performance Reduction of CO2 to Formate

作者：Guo, Weihua; Zhang, Yuefeng; Su, Jianjun; Song, Yun; Huang, Libei; Cheng, Le; Cao, Xiaohu; Dou, Yubing; Ma, Yangbo; Ma, Chenyan; Zhu, He; Zheng, Tingting; Wang, Zhaoyu; Li, Hao; Fan, Zhanxi; Liu, Qi; Zeng, Zhiyuan^*; Dong, Juncai; Xia, Chuan; Tang, Ben Zhong; Ye, Ruquan^*

来源：Small, 2022, 18(24): 2201311.

DOI：10.1002/smll.202201311

• abundant defects
• carbon dioxide reduction reaction
• industrial-relevance formate production rate
• laser activation
• low overpotential

Deficiencies in understanding the local environment of active sites and limited synthetic skills challenge the delivery of industrially-relevant current densities with low overpotentials and high selectivity for CO2 reduction. Here, a transient laser induction of metal salts can stimulate extreme conditions and rapid kinetics to produce defect-rich indium nanoparticles (L-In) is reported. Atomic-resolution microscopy and X-ray absorption disclose the highly defective and undercoordinated local environment in L-In. In a flow cell, L-In shows a very small onset overpotential of approximate to 92 mV and delivers a current density of approximate to 360 mA cm(-2) with a formate Faradaic efficiency of 98% at a low potential of -0.62 V versus RHE. The formation rate of formate reaches up to 6364.4 mu mol h(-1) mgIn-1$mg_{{\rm{In}}}<^>{--1}$, which is nearly 39 folds higher than that of commercial In (160.7 mu mol h(-1) mgIn-1$mg_{{\rm{In}}}<^>{--1}$), outperforming most of the previous results that have been reported under KHCO3 environments. Density function theory calculations suggest that the defects facilitate the formation of *OCHO intermediate and stabilize the *HCOOH while inhibiting hydrogen adsorption. This study suggests that transient solid-state laser induction provides a facile and cost-effective approach to form ligand-free and defect-rich materials with tailored activities.

• 单位
  电子科技大学; 中国科学院