{"title":"在银中空纤维气体扩散电极上设计界面分子相互作用,以实现二氧化碳到一氧化碳的高效转化。","authors":"Yizhu Kuang, Guoliang Chen, Dimuthu Herath Mudiyanselage, Hesamoddin Rabiee, Beibei Ma, Fatereh Dorosti, Ashok Kumar Nanjundan, Zhonghua Zhu, Hao Wang, Lei Ge","doi":"10.1002/chem.202403251","DOIUrl":null,"url":null,"abstract":"<p><p>The electrochemical CO2 reduction reaction (CO2RR) occurs at the nanoscale interface of the electrode-electrolyte. Therefore, tailoring the interfacial properties in the interface microenvironment provides a powerful strategy to optimise the activity and selectivity of electrocatalysts towards the desired products. Here, the microenvironment at the electrode-electrolyte interface of the flow-through Ag-based hollow fibre gas diffusion electrode (Ag HFGDE) is modulated by introducing surfactant cetyltrimethylammonium bromide (CTAB) as the electrolyte additive. The porous hollow fibre configuration and gas penetration mode facilitate the CO2 mass transfer and the formation of the triple-phase interface. Through the ordered arrangement of hydrophobic long-alkyl chains, CTAB molecules at the electrode/electrolyte interface promoted CO2 penetration to active sites and repelled water to reduce the activity of competitive hydrogen evolution reaction (HER). By applying CTAB-containing catholyte, Ag HFGDE achieved a high CO Faradaic efficiency (FE) of over 95 % in a wide potential range and double the partial current density of CO. The enhancement of CO selectivity and suppression of hydrogen was attributed to the improvement of charge transfer and the CO2/H2O ratio enhancement. These findings highlight the importance of adjusting the local microenvironment to enhance the reaction kinetics and product selectivity in the electrochemical CO2 reduction reaction CO2RR.</p>","PeriodicalId":144,"journal":{"name":"Chemistry - A European Journal","volume":null,"pages":null},"PeriodicalIF":3.9000,"publicationDate":"2024-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Engineering interfacial molecular interactions on Ag Hollow fibre gas diffusion electrodes for high efficiency in CO2 conversion to CO.\",\"authors\":\"Yizhu Kuang, Guoliang Chen, Dimuthu Herath Mudiyanselage, Hesamoddin Rabiee, Beibei Ma, Fatereh Dorosti, Ashok Kumar Nanjundan, Zhonghua Zhu, Hao Wang, Lei Ge\",\"doi\":\"10.1002/chem.202403251\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>The electrochemical CO2 reduction reaction (CO2RR) occurs at the nanoscale interface of the electrode-electrolyte. 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By applying CTAB-containing catholyte, Ag HFGDE achieved a high CO Faradaic efficiency (FE) of over 95 % in a wide potential range and double the partial current density of CO. The enhancement of CO selectivity and suppression of hydrogen was attributed to the improvement of charge transfer and the CO2/H2O ratio enhancement. 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引用次数: 0
摘要
电化学二氧化碳还原反应(CO2RR)发生在电极-电解质的纳米级界面上。因此,调整界面微环境中的界面特性为优化电催化剂对所需产物的活性和选择性提供了有力的策略。在这里,通过引入表面活性剂十六烷基三甲基溴化铵(CTAB)作为电解质添加剂,调节了流动式银基中空纤维气体扩散电极(Ag HFGDE)的电极-电解质界面微环境。多孔中空纤维结构和气体渗透模式促进了二氧化碳的传质和三相界面的形成。通过疏水性长烷基链的有序排列,CTAB 分子在电极/电解质界面上促进了二氧化碳向活性位点的渗透,并排斥水以降低竞争性氢进化反应(HER)的活性。通过使用含 CTAB 的阴极溶液,Ag HFGDE 在宽电位范围内实现了超过 95% 的高 CO 法拉第效率 (FE),并将 CO 的部分电流密度提高了一倍。一氧化碳选择性的提高和对氢的抑制归因于电荷转移的改善和 CO2/H2O 比率的提高。这些发现凸显了调整局部微环境对提高 CO2 还原反应 CO2RR 中的反应动力学和产物选择性的重要性。
Engineering interfacial molecular interactions on Ag Hollow fibre gas diffusion electrodes for high efficiency in CO2 conversion to CO.
The electrochemical CO2 reduction reaction (CO2RR) occurs at the nanoscale interface of the electrode-electrolyte. Therefore, tailoring the interfacial properties in the interface microenvironment provides a powerful strategy to optimise the activity and selectivity of electrocatalysts towards the desired products. Here, the microenvironment at the electrode-electrolyte interface of the flow-through Ag-based hollow fibre gas diffusion electrode (Ag HFGDE) is modulated by introducing surfactant cetyltrimethylammonium bromide (CTAB) as the electrolyte additive. The porous hollow fibre configuration and gas penetration mode facilitate the CO2 mass transfer and the formation of the triple-phase interface. Through the ordered arrangement of hydrophobic long-alkyl chains, CTAB molecules at the electrode/electrolyte interface promoted CO2 penetration to active sites and repelled water to reduce the activity of competitive hydrogen evolution reaction (HER). By applying CTAB-containing catholyte, Ag HFGDE achieved a high CO Faradaic efficiency (FE) of over 95 % in a wide potential range and double the partial current density of CO. The enhancement of CO selectivity and suppression of hydrogen was attributed to the improvement of charge transfer and the CO2/H2O ratio enhancement. These findings highlight the importance of adjusting the local microenvironment to enhance the reaction kinetics and product selectivity in the electrochemical CO2 reduction reaction CO2RR.
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