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Over a 15.9% Solar-to-CO Conversion from Dilute CO2 Streams Catalyzed by Gold Nanoclusters Exhibiting a High CO2 Binding Affinity
ACS Energy Letters ( IF 19.3 ) Pub Date : 2020-02-14 , DOI: 10.1021/acsenergylett.9b02511
Beomil Kim 1 , Hoeun Seong 2 , Jun Tae Song 3 , Kyuju Kwak 2 , Hakhyeon Song 1 , Ying Chuan Tan 1 , Gibeom Park 2 , Dongil Lee 2 , Jihun Oh 1, 3
Affiliation  

Development of efficient and selective electrocatalysts is a key challenge to achieve an industry-relevant electrochemical CO2 reduction reaction (CO2RR) to produce commodity chemicals. Here, we report that Au25 clusters with Au-thiolate staple motifs can initiate electrocatalytic reduction of CO2 to CO with nearly zero energy loss and achieve a high CO2RR current density of 540 mA cm–2 in a gas-phase reactor. Electrochemical kinetic investigations revealed that the high CO2RR activity of the Au25 originates from the strong CO2 binding affinity, leading to high CO2 electrolysis performance in both concentrated and dilute CO2 streams. Finally, we demonstrated an 18.0% solar-to-CO conversion efficiency using a Au25 electrolyzer powered by a Ga0.5In0.5P/GaAs photovoltaic cell. The electrolyzer also showed 15.9% efficiency and a 5.2% solar-driven single-path CO2 conversion rate in a 10% CO2 gas stream, the CO2 concentration in a typical flue gas.

中文翻译:

具有高CO 2结合亲和力的金纳米团簇催化稀CO 2流产生的太阳能转化为CO的转化率超过15.9%

有效和选择性的电催化剂的开发是实现与工业相关的电化学CO 2还原反应(CO 2 RR)来生产商品化学品的关键挑战。在这里,我们报道Au-硫醇盐钉基序的Au 25簇可以在几乎零能量损失的情况下将CO 2电催化还原为CO ,并在气相反应器中实现540 mA cm –2的高CO 2 RR电流密度。电化学动力学研究表明,Au 25的高CO 2 RR活性源自强大的CO 2结合亲和力,导致高CO 2在浓和稀的CO 2流中的电解性能。最后,我们证明了使用由Ga 0.5 In 0.5 P / GaAs光伏电池供电的Au 25电解槽,太阳能转化为CO的效率为18.0%。在10%CO 2气流中,该电解槽还显示出15.9%的效率和5.2%的太阳能驱动的单路径CO 2转化率,即典型烟道气中的CO 2浓度。
更新日期:2020-02-17
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