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CO2 electroreduction to formate is technically feasible and economically viable, but still suffers from low selectivity and high overpotential at industrial current densities. Here, lattice-distorted metallic nanosheets with disorder-engineered metal sites are designed for industrial-current-density CO2-to-formate conversion at low overpotentials. As a prototype, richly lattice-distorted bismuth nanosheets are first constructed, where abundant disorder-engineered Bi sites could be observed by high-angle annular dark-field scanning transmission electron microscopy image. In-situ Fourier-transform infrared spectra reveal the CO2•−* group is the key intermediate, while theoretical calculations suggest the electron-enriched Bi sites could effectively lower the CO2 activation energy barrier by stabilizing the CO2•−* intermediate, further affirmed by the decreased formation energy from 0.49 to 0.39 eV. As a result, the richly lattice-distorted Bi nanosheets exhibit the ultrahigh current density of 800 mA·cm−2 with 91% Faradaic efficiencies for CO2-to-formate electroreduction, and the formate selectivity can reach nearly 100% at the current density of 200 mA·cm−2 with a very low overpotential of ca. 570 mV, outperforming most reported metal-based electrocatalysts.
This work was financially supported by the National Key Research and Development Program of China (No. 2019YFA0210004), the National Natural Science Foundation of China (Nos. 22125503, 21975242, U2032212, and 21890754), the Strategic Priority Research Program of Chinese Academy of Sciences (No. XDB36000000), Youth Innovation Promotion Association of CAS (No. CX2340007003), the Key Research Program of Frontier Sciences of CAS (No. QYZDY-SSW-SLH011), the Major Program of Development Foundation of Hefei Center for Physical Science and Technology (No. 2020HSC-CIP003), Users with Excellence Program of Hefei Science Center CAS (No. 2020HSC-UE001), and the University Synergy Innovation Program of Anhui Province (No. GXXT-2020-001). Supercomputing University of Science and Technology of China (USTC) and the National Supercomputing Center in Shenzhen are acknowledged for computational support.