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Syngas (CO + H2) is the incredibly important feedstock for producing synthetic fuels and various value-added chemicals. CO2 electrochemical reduction to syngas is an environmental-friendly and sustainable approach, but still challenging to produce tunable syngas with a wide ratio of CO/H2. Herein, by modulating the structure and phase, we have successfully obtained a series of copper–indium (Cu-In) catalysts, which are efficient for producing syngas with tunable CO/H2 ratios. A series of CuIn bimetallic catalysts with different structures from hollow sphere to two-layer hollow sphere and different phases from CuO to Cu2O are developed. We find that the CO and H2 are the only gaseous products, in which the CO/H2 ratios can be readily tuned from 1.2 ± 0.1 to 9.0 ± 1.5 by simply controlling the thermal annealing temperature. It also exhibits high durability during a 10-h test. The unique performance is attributed to the modulated In enrichment on the Cu surfaces during the CO2 reduction reaction, which causes the differences in binding energies for key reaction intermediates, thus resulting in the tunable composition of syngas. The present work emphasizes a simple yet efficient phase and structure modulating strategy for designing potential electrocatalysts for producing syngas with widely tunable CO/H2 ratios.
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