The electrocatalytic carbon dioxide reduction reaction (CO2RR) addresses the need for storage of renewable energy in valuable carbon-based fuels and feedstocks, yet challenges remain in the improvement of electrosynthesis pathways for highly selective hydrocarbon production. To improve catalysis further, it is of increasing interest to lever synergies between heterogeneous and homogeneous approaches. Organic molecules or metal complexes adjacent to heterogeneous active sites provide additional binding interactions that may tune the stability of intermediates, improving catalytic performance by increasing Faradaic efficiency (product selectivity), as well as decreasing overpotential. We offer a forward-looking perspective on molecularly enhanced heterogeneous catalysis for CO2RR. We discuss four categories of molecularly enhanced strategies: molecular-additive-modified heterogeneous catalysts, immobilized organometallic complex catalysts, reticular catalysts and metal-free polymer catalysts. We introduce present-day challenges in molecular strategies and describe a vision for CO2RR electrocatalysis towards multi-carbon products. These strategies provide potential avenues to address the challenges of catalyst activity, selectivity and stability in the further development of CO2RR.

中文翻译：

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降低非均相二氧化碳的分子增强。

电催化二氧化碳还原反应（CO2RR）满足了将可再生能源存储在有价值的碳基燃料和原料中的需求，但是在改善高选择性碳氢化合物生产的电合成途径方面仍然存在挑战。为了进一步改善催化作用，利用异质和均相方法之间的协同作用越来越引起人们的兴趣。与异质活性位点相邻的有机分子或金属络合物提供了额外的键合相互作用，可以调节中间体的稳定性，通过提高法拉第效率（产物选择性）以及降低过电势来改善催化性能。我们提供了分子增强的CO2RR多相催化的前瞻性观点。我们讨论了分子增强策略的四类：分子添加剂改性的多相催化剂，固定化的有机金属络合物催化剂，网状催化剂和无金属的聚合物催化剂。我们介绍了分子策略中的当今挑战，并描述了CO2RR电催化制备多碳产品的愿景。这些策略提供了潜在的途径来解决在CO2RR进一步发展中催化剂活性，选择性和稳定性的挑战。