摘要
Tandem catalysis,capable of decoupling individual steps,provides a feasible way to build a high-efficiency CO_(2) electro-conversion system for multicarbons(C_(2+)).The construction of electrocatalytic materials is one of focusing issues.Herein,we fabricated a single atom involved multivalent oxide-derived Cu composite material and found it inclined to reconstruct into oxygen-deficient multiphase Cu based species hybridized with monatomic Ni on N doped C matrix.In this prototype,rapid CO generation and C-C coupling are successively achieved on NiN4 sites and surface amorphized Cu species with defects,resembling a micro-production line.In this way,the in situ formed tandem catalyst exhibited a high Faradaic efficiency(FE)of~78%for C_(2+)products along with satisfactory durability over 50 h.Particularly,the reconstruction-induced amorphous layer with abundant asymmetric sites should be favorable to improve the ethanol selectivity(FE:63%),which is about 10 times higher than that of the non-tandem Cu-based contrast material.This work offers a new approach for manipulating tandem catalyst systems towards enhancing C_(2+)products.
基金
supported by the National Natural Science Foundation of China(Nos.52302092,22375019)
the Beijing Natural Science Foundation(No.2212018)
the Beijing Institute of Technology Research Fund Program for Young Scholars(No.2022CX01011)
the Fundamental Research Funds for the Central Universities(Nos.2023MS057 and JB 2022004)
the Open Research Fund of State Environmental Protection Key Laboratory of Eco-industry,Chinese Research Academy of Environmental Sciences(No.2022KFF-07).