Atomically dispersed Ni catalyst to boost weak sunlight-driven CO2 hydrogenation with 100% CO selectivity

Ni based catalysts are highly stable and active for CO2 hydrogenation as CO, but the CO selectivity can not reach 100 %, which has not been realized so far. In this work, theoretical calculations are used to predict that Ni single atoms can cause Pauli incompatibility to block the CH4 production path of CO2 hydrogenation, so as to achieve 100 % CO produced selectivity of Ni based catalysts. Based on theoretical prediction, Ni single atoms supported on CeO2 nanosheets (SA Ni/CeO2) are synthesized for CO2 hydrogenation, which displays a high CO production rate of 47.06 mmol·g−1·h−1 at 500 °C and an unprecedented 100 % CO selectivity. Further, the SA Ni/CeO2 supported by homemade solar heating conversion device exhibits a CO production rate of 23.1 mmol·g−1·h−1 with 100 % CO selectivity from the solar heating CO2 hydrogenation under 3 suns irradiation, 4.7 times higher than the record of weak sunlight driven CO production.