机构地区:[1]东华大学材料科学与工程学院,纤维材料改性国家重点实验室,上海201620 [2]宁波工程学院新能源学院,浙江宁波315336
出 处:《中国粉体技术》2025年第2期81-90,共10页China Powder Science and Technology
基 金:国家自然科学基金项目,编号:52272289。
摘 要:【目的】梳理(electrocatalytic CO_(2) reduction reaction,eCO_(2)RR)的金属颗粒催化剂的设计策略,探讨其用于酸性介质中对电催化二氧化碳还原反应的影响。【研究现状】综述用于酸性eCO_(2)RR的金属催化剂设计策略,大体分为双金属催化、非金属元素掺杂、形貌调控、有机物修饰、无机层修饰金属颗粒策略;双金属催化策略是实现催化剂对反应底物及中间体选择性吸附的有效方法,更利于活性位的暴露,在实现大电流密度电解上有一定优势;非金属元素掺杂策略在优化中间体吸附、提高酸性eCO_(2)RR产物选择性方面具有很大潜力;颗粒大小、晶界、空位及晶面等影响底物与中间体吸附强度的形貌因素都可对酸性eCO_(2)RR产物分布产生影响;有机物修饰策略大多基于在金属催化剂表面富集碱金属离子,高浓度碱金属盐易析出并沉积,影响催化稳定性;无机物修饰金属颗粒策略主要在金属颗粒外包裹疏水性碳层、SiO_(2)等无机物,以提高酸性eCO_(2)RR选择性。【结论与展望】提出催化剂颗粒的分级结构设计、界面、表面工程及电子结构调控等方法在降低eCO_(2)RR过电位、提高反应速率、产物选择性及催化稳定性方面潜力巨大;认为促进酸性eCO_(2)RR应用化发展要进一步明确特定产物的形成及调控机制,创新催化剂颗粒结构。Significance To review the design strategies for metal particle catalysts used in the electrocatalytic CO_(2) reduction reaction(eCO_(2)RR)in acidic media and to support further development of acidic eCO_(2)RR research.Progress This review summarizes recent reports on the structural design methods of catalyst particles for acidic eCO_(2)RR.The cur-rent design methods for metal catalysts used in acidic eCO_(2)RR can be broadly categorized into organic modification,bimetallic cataly-sis,non-metal element doping,inorganic layer modification,and morphology control.The increased concentration of H+in acidic electrolytes raises the surface-adsorbed H+(*H)ratio on the electrode,enhancing hydrogen evolution reaction(HER)kinetics,which in turn leads to poor product selectivity and low activity in acidic eCO_(2)RR.Reducing the local H+concentration on the elec-trode surface or increasing the adsorption selectivity of the electrode material for CO_(2) and intermediates are potential methods for pro-moting acidic eCO_(2)RR.Conclusions and Prospects In 2021,acidic eCO_(2)RR was first proposed.Over the past few years,some catalysts have achieved high product selectivity in acidic eCO_(2)RR,yet significant challenges remain:1)A method that simultaneously achieves high selectivity,high reaction rates,and high stability in acidic eCO_(2)RR is still lacking.Current designs for acidic catalysts often rely on alkali metal ions(e.g.,K⁺)to suppress HER and activate CO_(2).However,these designs typically require the addition of high concentrations of alkali metal salts,which can lead to salt deposition,impairing gas diffusion and catalytic stability.Additionally,non-precious metal catalysts tend to dissolve in acidic media,resulting in active site loss.Encapsulating the exterior of metal particles with suitable organic or inorganic layers can improve catalytic stability to some extent but may block active sites,thereby reducing the conversion rate.2)The selectivity for single multi-electron transfer products in acidic eCO_(2)RR needs
关 键 词:电催化CO_(2)还原反应 酸性介质 表面微环境 电子结构 催化剂设计
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