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We developed an approach to realize the comprehensive utilization of CO2 and glycerol by smartly design a nanocatalyst, which concerns the coupling of catalytic reactions and the separation or capture process. Specifically, MgFe‐CO32−‐LDHs with different thickness were fabricated by employing atmospheric CO2 as carbon source and an atomic‐level interface was constructed by introducing Pt single atoms to obtain series of Pt/MgFe‐LDHs nanocatalysts. During a catalytic assessment, the CO32− confined within interlayer was in situ converted when integrated with glycerol oxidation under irradiation. The optimal nanocatalyst exhibited a decent conversion efficiency of CO32−‐CO‐CH4 and near 100% selectivity of secondary hydroxy group in glycerol. DFT calculation, isotope‐labeled experiments and in situ spectrograph characterization revealed possible coupling reaction mechanism. More importantly, the nanocatalyst exhibited impressive reusability for at least six 6 runs. The developed multiple coupling process will be an alternative and promising procedure for the waste and low‐valued sources synergetic utilization. [ABSTRACT FROM AUTHOR]

We reported a strategy of carbon‐negative H2 production in which CO2 capture was coupled with H2 evolution at ambient temperature and pressure. For this purpose, carbonate‐type CuxMgyFez layered double hydroxide (LDH) was preciously constructed, and then a photocatalysis reaction of interlayer CO32− reduction with glycerol oxidation was performed as driving force to induce the electron storage on LDH layers. With the participation of pre‐stored electrons, CO2 was captured to recover interlayer CO32− in presence of H2O, accompanied with equivalent H2 production. During photocatalysis reaction, Cu0.6Mg1.4Fe1 exhibited a decent CO evolution amount of 1.63 mmol g−1 and dihydroxyacetone yield of 3.81 mmol g−1. In carbon‐negative H2 production process, it showed an exciting CO2 capture quantity of 1.61 mmol g−1 and H2 yield of 1.44 mmol g−1. Besides, this system possessed stable operation capability under simulated flu gas condition with negligible performance loss, exhibiting application prospect. [ABSTRACT FROM AUTHOR]

We reported a strategy of carbon‐negative H2 production in which CO2 capture was coupled with H2 evolution at ambient temperature and pressure. For this purpose, carbonate‐type CuxMgyFez layered double hydroxide (LDH) was preciously constructed, and then a photocatalysis reaction of interlayer CO32− reduction with glycerol oxidation was performed as driving force to induce the electron storage on LDH layers. With the participation of pre‐stored electrons, CO2 was captured to recover interlayer CO32− in presence of H2O, accompanied with equivalent H2 production. During photocatalysis reaction, Cu0.6Mg1.4Fe1 exhibited a decent CO evolution amount of 1.63 mmol g−1 and dihydroxyacetone yield of 3.81 mmol g−1. In carbon‐negative H2 production process, it showed an exciting CO2 capture quantity of 1.61 mmol g−1 and H2 yield of 1.44 mmol g−1. Besides, this system possessed stable operation capability under simulated flu gas condition with negligible performance loss, exhibiting application prospect. [ABSTRACT FROM AUTHOR]