4.6 Article

Photoelectrochemical reduction of CO2 catalyzed by a 3D core-shell NiMoO4@ZnO heterojunction with bicentre at the (111) plane and thermal electron assistance

Journal

JOURNAL OF MATERIALS CHEMISTRY A
Volume 11, Issue 8, Pages 4230-4237

Publisher

ROYAL SOC CHEMISTRY
DOI: 10.1039/d2ta09055d

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The photoelectrochemical reduction of CO2 into organic chemicals on a semiconductor is a feasible solution to the global energy crisis and climate warming. In this study, NiMoO4/ZnO-x heterojunctions were designed and synthesized. The nanosheets of NiMoO4 have high photon absorption and promote the coupling of C-C to generate C2 compounds. The ZnO/C core, fabricated from MOF rich in CN species, generates thermal electrons to assist CO2 reduction.
The photoelectrochemical (PEC) reduction of CO2 into organic chemicals on the semiconductor is considered a feasible plan to address the global energy crisis and climate warming. Herein, the heterojunctions NiMoO4/ZnO-x are designed and synthesized. The nanosheets of NiMoO4 have excellent absorption of photons and benefit the C-C coupling to C2 compounds. The ZnO/C core fabricated from MOF rich in CN species harvests light to generate a lot of thermal electrons assisting CO2 reduction. Benefitting from its unique chemical properties and structure, the as-prepared NiMoO4/ZnO-3 heterojunction exhibited impressive performance in CO2 reduction, yielding oxygenated chemicals with 72.6% selectivity for C2 products at a rate of 29.2 mu M cm(-2) h(-1). The formation rate under photoelectrochemical conduction is three times that of photocatalysis plus electrocatalysis, showing a strong synergetic effect of photo- and electro-catalysis. The isotopic labeling experiments of (CO2)-C-13 verified that the products are derived from CO2 and water. Finally, a new catalytic mechanism with bimetallic centers is proposed firstly to explain the reaction pathways with high selectivity of C2 chemicals. The important intermediates and the C-C coupling via Ni-Mo bicentre are proven by density-functional theory (DFT) calculations and verified by operando Fourier transform infrared (FTIR) spectrometry. On the other hand, the effect of thermal electrons is investigated as well.

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