Highly efficient solar-driven CO2-to-fuel conversion assisted by CH4 over NiCo-ZIF derived catalysts

• Published in: Fuel (Guildford) 2022-02, Vol.310, p.122441, Article 122441
• Main Authors: Liu, Xianglei, Mu, Zekai, Sun, Chen, Shi, Hang, Meng, Xianguang, Li, Ping, Ling, Yueyue, Cheng, Bo, Xuan, Yimin, Ding, Yulong
• Format: Article
• Language: English
• Subjects: Aluminum oxide; Bimetals; Carbon dioxide; Catalysts; Climate change; CO2 reduction; Conversion; Deactivation; Dry reforming of methane; Energy efficiency; Energy shortages; Fuel consumption; Fuel economy; Global warming; Greenhouse effect; Greenhouse gases; Intermetallic compounds; Light; Low temperature; Metal particles; Methane; Nanostructure; NiCo alloy; Operating temperature; Solar fuel; Ultrahigh temperature; ZIF
• ISSN: 0016-2361; 1873-7153
• DOI: 10.1016/j.fuel.2021.122441

The light-to-fuel efficiency achieves a record-high value of 32.4% with operation temperature below 600 °C (594 °C) via NiCo-ZIF derived catalysts. [Display omitted] •A novel NiCo alloy nanocatalyst is designed for direct solar-driven CO2-to-fuel conversion assisted by CH4.•NiCo catalyst shows unique synergetic catalysis effect with low carbon deposition.•NiCo catalyst exhibits photo-enhanced CO2 reduction activity with low activation energy.•An ultrahigh light-to-fuel efficiency of 32.4% with operation temperature below 600 °C is achieved. Solar-driven CO2 reduction by CH4 is promising to simultaneously tackle energy shortage and global warming problems by converting two greenhouse gases into fuels. However, serious challenges remain, such as limited light-to-fuel efficiency, high operating temperature, and severe catalyst deactivation. Here, high-performance direct solar-driven CO2 reduction is demonstrated at relatively low operation temperature (594 °C) based on NiCo-ZIF derived nanostructures. An ultrahigh light-to-fuel efficiency of 32.4% and production rates of H2 (105.83 min−1g−1) and CO (128.17 mmol min−1g−1) are achieved via photothermocatalysis on Ni1Co2@CZIF-Al2O3 catalysts. Excellent light-to-fuel conversion performance can be attributed to the highly dispersed metal particles, decreased apparent activation energy under direct light illumination, increased CO2 absorption, and promoted dissociation of CH4 to CH3* of NiCo alloy. The carbon deposition rate of NiCo bimetallic catalysts is prominently inhibited compared with pure Ni or Co catalysts due to the change of the reaction path, as confirmed by DFT calculations. This work opens new routes to achieve highly efficient solar-driven CO2 reduction by CH4 based on NiCo-ZIF derived alloy nanostructures at relatively low-temperature conditions.