Research Progress on Triphase Interface Electrocatalytic Carbon Dioxide Reduction

Abstract

Electrocatalytic carbon dioxide reduction is the focus and nodus of energy chemistry and catalytic science. As a basic concept in physical chemistry, gas-solid-liquid triphase interface model has been widely studied in electrocatalytic carbon dioxide reduction reaction in recent years, showing many advantages compared with traditional solid-liquid biphase systems. In this review, we discuss the research progress of triphase interface eletrocatalytic carbon dioxide reduction, focused on the classification as well as the principle of triphase interface eletrocatalytic systems. Then, carbon dioxide electroreduction properties of various triphase systems including underwater superaerophilic and gas diffusion layer systems are discussed, with special attention on the influence factors, such as the interfacial diffusion and interfacial wettability of reactants. Finally, we summarize and prospect the existing problems and the future development direction of electrocatalytic carbon dioxide reduction based on triphase systems. Keywords triphase interface; carbon dioxide reduction; electrocatalysis; mass transfer; wettability 1 引言 随着社会飞速发展, 能源过度消耗以及温室气体大 量排放已成为严峻的环境问题 [1] . 二氧化碳(CO 2 )是温 室气体中的主要成分, 然而基于自然界植物光合作用的 碳循环过程已无法抵消人类活动所排放的 CO 2 . 因此, 发展清洁、高效的人工固碳技术成为了目前能源与环境 领域的研究重点 [2][3][4][5] . 在众多 CO 2 转化策略中, 电催化 CO 2 还原策略(电力来源于可再生能源, 如太阳能、风 能、潮汐能等)能够在室温常压下将 CO 2 分子高选择性 地还原为清洁燃料或高附加值化学品 [6][7] , 被认为是一 项能够缓解能源与环境问题的"一箭双雕"的未来技术. 电催化 CO 2 还原反应的效率通常取决于两个方面: (1) CO 2 分子在催化剂表面的多步质子辅助电子转移过 程 [8] ; (2) CO 2 等反应物的界面扩散传质动力学过程 [9] . 其中, 前者主要受催化材料的晶体结构和活性位组成影 响, 而后者受催化反应界面结构、浸润性等的物理化学 性质影响. 其中, 关于催化材料组分结构调控方面的研 究已经取得了丰富的研究成果, 能够在较小的电流密度 下实现极高的 CO 2 还原产物选择性. 然而, 在传统的固-液两相反应体系中, CO 2 需要先溶解在电解液中, 再经 历液相扩散过程至电极界面参与反应. 但是 CO 2 在电解 液中的溶解度偏小且液相扩散系数极低 [10] , 导致 CO 2 还 原的电流密度无法有效提升, 同时加剧了析氢反应

Nickel-Nitrogen-Doped Ordered Macro-/Mesoporous Carbon Supported Ag Nanoparticles for Efficient Electrocatalytic CO2Reduction

“…为了缓解全球对化石燃料的依赖并应对化石燃料 燃烧产生的高浓度 CO 2 导致的气候问题, 科研工作者们 开发了电催化 [1][2][3] 、 光催化 [4][5] 、 生物催化 [6] 和有机合成 [7][8] 等技术对 CO 2 进行催化转化, 以降低大气中的 CO 2 浓 度. 电催化还原 CO 2 技术(ECR), 由于其可以以太阳能、 风能等可再生能源作为动力, 将 CO 2 转化为高附加值的 化学产品(如 CO、HCOOH 以及其他 C 2＋ 产物等), 受到 了诸多研究者的青睐 [9] . 相比于其他产物, 将 CO 2 还原 为 CO 机理简单, 其产物更容易从电解质中分离, 被认 为是最有希望实现商业化的办法 [10][11] .…”

Two-dimensional materials: synthesis and applications in the electro-reduction of carbon dioxide

“…2D structures, such as nanoplates, nanosheets, and nanoflakes, have been using for preparation of various materials, including metals, metal oxides, metallic sulfides, and carbon materials [41][42][43][44] . Until now, numerous 2D materials have been designed and prepared for CO 2 electro-reduction [45][46][47] . For commercial applications of electrocatalysts, high yield and controllable fabrication techniques are essential.…”

Challenges and prospects of lithium–CO2batteries

“…4(b))[55][56][57]. Having a clearer identification of the interfacial mechanisms for better reorganization and designation of Li-CO2 batteries is quite significant.…”