SanHe Power Plant Ltd.,CHN Energy
National Energy Research and Development Center of Carbon Capture
Hebei Province Coal-fired Power Station Pollution Prevention and ControlTechnology Innovation Center
State Key Laboratory of Coal Combustion,Huazhong University ofScience and Technology

碳达峰、碳中和是实现我国绿色可持续发展发展的重大战略需求。合成气作为现代化工生产的重要基础原料,其传统的制备方法高度依赖化石能源,导致了大量的温室气体排放利用可再生电力驱动的电催化CO2还原制合成气技术作为一种环保且可持续的替代方案,近年来受到广泛的研究与关注。虽然已有研究探讨了不同催化剂对电催化CO2还原制合成气的V(H2)/V(CO)的影响,但对于在单一催化剂上实现对合成气产物中H2和CO选择性的有效调控仍具有挑战性。为了实现在单一催化剂上对合成气产物中V(H2)/V(CO)的选择性调控,本研究采用高温固相合成工艺合成了CuGa2金属间化合物,用以作为电催化剂来实现高选择性、可调性电催化CO2还原制合成气,并通过SEM、EDS、XRD和XPS等一系列表征分析手段,研究了CuGa2金属间化合物的理化特性与电化学性能,并探究了CuGa2金属间化合物在电催化CO₂还原过程中的相关催化机理。研究结果表明,该催化剂作为CuGa2和少量金属氧化物的混合物,能够通过改变电解液浓度、调控pH值的手段,显著调控其对于电催化CO2还原反应(eCO2RR)和析氢反应(HER)的选择性,从而调控合成气产物中的V(H2)/V(CO)。此外,不同电位对V(H2)/V(CO)的影响测试结果显示,通过控制施加电位,可以调节CuGa2催化剂活性位点的利用率,进而改变eCO2RR和HER的选择性,实现合成气产物中V(H2)/V(CO)在0.3~4内可调。

Achieving carbon peak and carbon neutrality is a critical strategic requirement for China's green and sustainable development.Syngas,as a vital raw material for modern chemical production,traditionally relies heavily on fossil fuels for its preparation,resulting insignificant greenhouse gas emissions. In recent years, the technology of electrocatalytic CO2 reduction to syngas driven by renewableelectricity has emerged as an environmentally friendly and sustainable alternative,garnering extensive research interest.While previousstudies have explored the impact of different catalysts on the V(H2)/V(CO) ratio in syngas produced via electrocatalytic CO2 reduction,effectively tuning the selectivity of H2 and CO using a single catalyst remains a challenge. To achieve selective modulation of the V(H2) /V(CO) ratio in syngas products with a single catalyst,this study synthesized CuGa2 intermetallic compounds through a high-temperaturesolid-state synthesis process. These compounds were employed as electrocatalysts to enable high selectivity and tunability in theelectrocatalytic CO2 reduction to syngas.A range of characterization techniques, including SEM, EDS, XRD, and XPS, were used toinvestigate the physicochemical properties and electrochemical performance of the CuGa2 intermetallics, as well as their catalytic mechanisms during the electrocatalytic CO2 reduction process. The results indicated that this catalyst,consisting of a mixture of CuGa2and a small amount of metal oxides,could significantly adjust its selectivity for the electrocatalytic CO2 reduction reaction (eCO2RR) and the hydrogen evolution reaction (HER) by varying electrolyte concentration and pH,thereby modulating the V(H2)/V(CO) ratio in the syngas produced.Moreover,tests examining the impact of different applied potentials on the V(H2)/V(CO) ratio demonstrated that controlling the applied potential allows for the adjustment of active site utilization in the CuGa2 catalyst,thus altering the selectivity of both eCO2RR and HER. This enables the V(H2)/V(CO) ratio in syngas products to be tuned within a range of 0.3 to 4.

湖北省重点研发资助项目(2021BCD003),河北省重点研发资助项目(22373708D)

张军峰,魏书洲,王畅,等.CuGa2电催化CO2还原制合成气[J].洁净煤技术,2024,30(11):97−103.

ZHANG Junfeng,WEI Shuzhou,WANG Chang,et al. CO2 reduction to syngas by CuGa2 electrocatalysis[J].Clean Coal Technology,2024,30(11):97−103.