Citation: Xudong Lv, Tao Shao, Junyan Liu, Meng Ye, Shengwei Liu. 电催化CO2还原耦合HCHO氧化反应系统促进污染物同步经济高效资源化转化[J]. Acta Physico-Chimica Sinica, ;2024, 40(5): 230502. doi: 10.3866/PKU.WHXB202305028
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传统电化学CO2还原(CO2RR)系统中阳极发生的水氧化半反应(WOR)具有动力学缓慢、过电位大、能耗高等缺点,限制了CO2RR系统的经济效益和应用。因此,本研究引入MnO2阳极进行甲醛氧化半反应(FOR)以代替WOR,构建了一种新型CO2RR/FOR耦合系统。与传统的CO2RR/WOR系统相比,在相同的施加电势下,CO2RR/FOR耦合系统的CO2RR电流密度和CO2RR产物的生成速率通常更具有优势。此外,在CO2RR/FOR耦合系统中,在合适的施加电势下,HCHO可以选择性地转化为HCOOH。具体来说,两电极CO2RR/FOR耦合系统中,在3.5 V的槽电压下,近90%的HCHO可以被去除,且HCHO会选择性转化为HCOOH,其转化率约为48%。更重要的是,在不同的工作电流下,FOR所需的电势比WOR所需的电势要小。在-10 mA·cm-2时,CO2RR/FOR耦合系统能降低约210 mV的槽电压,并且其能耗比单独的CO2RR系统和FOR系统的能耗之和降低45.13%。值得注意的是,当使用商业多晶硅太阳能电池作为电源时,在CO2RR/FOR耦合系统中的CO2RR电流密度、CO2RR产物的生成速率和HCHO到HCOOH的选择性仍然可以实现相当的改善。目前的工作将进一步推动研究开发新型的CO2RR耦合系统,以经济有效地将CO2和有机污染物同时转化为有价值的化学品。
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Keywords:
- CO2 reduction,
- HCHO oxidation,
- Paired electrochemical system,
- Cu,
- MnO2
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