Insights into the Low Overpotential Electroreduction of CO2 to CO on a Supported Gold Catalyst in an Alkaline Flow Electrolyzer,ACS Energy Letters

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Insights into the Low Overpotential Electroreduction of CO2 to CO on a Supported Gold Catalyst in an Alkaline Flow Electrolyzer
ACS Energy Letters ( IF 19.3 ) Pub Date : 2017-12-18 00:00:00 , DOI: 10.1021/acsenergylett.7b01096
Sumit Verma _{1,

2} , Yuki Hamasaki _{2,

3} , Chaerin Kim _{2,

3} , Wenxin Huang _{2,

3} , Shawn Lu ₁ , Huei-Ru Molly Jhong _{1,

2} , Andrew A. Gewirth _{2,

4} , Tsuyohiko Fujigaya _{2,

3} , Naotoshi Nakashima _{2,

3} , Paul J. A. Kenis _{1,

2}

Affiliation

Cost competitive electroreduction of CO₂ to CO requires electrochemical systems that exhibit partial current density (j_CO) exceeding 150 mA cm^–2 at cell overpotentials (|η_cell|) less than 1 V. However, achieving such benchmarks remains difficult. Here, we report the electroreduction of CO₂ on a supported gold catalyst in an alkaline flow electrolyzer with performance levels close to the economic viability criteria. Onset of CO production occurred at cell and cathode overpotentials of just −0.25 and −0.02 V, respectively. High j_CO (∼99, 158 mA cm^–2) was obtained at low |η_cell| (∼0.70, 0.94 V) and high CO energetic efficiency (∼63.8, 49.4%). The performance was stable for at least 8 h. Additionally, the onset cathode potentials, kinetic isotope effect, and Tafel slopes indicate the low overpotential production of CO in alkaline media to be the result of a pH-independent rate-determining step (i.e., electron transfer) in contrast to a pH-dependent overall process.

中文翻译：

碱性流动电解槽中负载型金催化剂上将CO ₂低电位电还原为CO的见解

CO的成本竞争力的电还原₂至CO需要表现出局部电流密度（电化学系统Ĵ _CO）超过150毫安厘米^-2在细胞的超电势（|η_细胞|）小于1 V.然而，实现这样的基准仍然是困难的。在这里，我们报告了在碱性流电解槽中负载型金催化剂上的CO ₂的电还原性能水平接近经济可行性标准。一氧化碳的产生分别发生在电池和阴极的过电势分别为-0.25和-0.02 V的时候。高Ĵ _CO（〜99，158毫安厘米^-2在低获得）|η_细胞| （〜0.70，0.94 V）和高的CO能量效率（〜63.8，49.4％）。性能稳定至少8小时。另外，开始的阴极电势，动力学同位素效应和Tafel斜率表明，在碱性介质中CO低的超电势产生是pH依赖性速率确定步骤（即电子转移）的结果，而不是pH依赖性整个过程。

更新日期：2017-12-18

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