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Selective CO2 Reduction to CO in Water using Earth-Abundant Metal and Nitrogen-Doped Carbon Electrocatalysts
ACS Catalysis ( IF 11.3 ) Pub Date : 2018-06-12 00:00:00 , DOI: 10.1021/acscatal.8b01022 Xin-Ming Hu 1, 2 , Halvor Høen Hval 1, 2 , Emil Tveden Bjerglund 1, 2 , Kirstine Junker Dalgaard 2 , Monica Rohde Madsen 1, 2 , Marga-Martina Pohl 3 , Edmund Welter 4 , Paolo Lamagni 1, 2 , Kristian Birk Buhl 1, 2 , Martin Bremholm 2 , Matthias Beller 3 , Steen Uttrup Pedersen 1, 2 , Troels Skrydstrup 1, 2 , Kim Daasbjerg 1, 2
ACS Catalysis ( IF 11.3 ) Pub Date : 2018-06-12 00:00:00 , DOI: 10.1021/acscatal.8b01022 Xin-Ming Hu 1, 2 , Halvor Høen Hval 1, 2 , Emil Tveden Bjerglund 1, 2 , Kirstine Junker Dalgaard 2 , Monica Rohde Madsen 1, 2 , Marga-Martina Pohl 3 , Edmund Welter 4 , Paolo Lamagni 1, 2 , Kristian Birk Buhl 1, 2 , Martin Bremholm 2 , Matthias Beller 3 , Steen Uttrup Pedersen 1, 2 , Troels Skrydstrup 1, 2 , Kim Daasbjerg 1, 2
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Earth-abundant transition metal (Fe, Co, or Ni) and nitrogen-doped porous carbon electrocatalysts (M-N-C, where M denotes the metal) were synthesized from cheap precursors via silica-templated pyrolysis. The effect of the material composition and structure (i.e., porosity, nitrogen doping, metal identity, and oxygen functionalization) on the activity for the electrochemical CO2 reduction reaction (CO2RR) was investigated. The metal-free N-C exhibits a high selectivity but low activity for CO2RR. Incorporation of the Fe and Ni, but not Co, sites in the N-C material is able to significantly enhance the activity. The general selectivity order for CO2-to-CO conversion in water is found to be Ni > Fe ≫ Co with respect to the metal in M-N-C, while the activity follows Ni, Fe ≫ Co. Notably, the Ni-doped carbon exhibits a high selectivity with a faradaic efficiency of 93% for CO production. Tafel analysis shows a change of the rate-determining step as the metal overtakes the role of the nitrogen as the most active site. Recording the X-ray photoelectron spectra and extended X-ray absorption fine structure demonstrates that the metals are atomically dispersed in the carbon matrix, most likely coordinated to four nitrogen atoms and with carbon atoms serving as a second coordination shell. Presumably, the carbon atoms in the second coordination shell of the metal sites in M-N-C significantly affect the CO2RR activity because the opposite reactivity order is found for carbon supported metal meso-tetraphenylporphyrin complexes. From a better understanding of the relationship between the CO2RR activity and the material structure, it becomes possible to rationally design high-performance porous carbon electrocatalysts involving earth-abundant metals for CO2 valorization.
中文翻译：
使用富含地球的金属和掺氮的碳电催化剂选择性还原水中的CO 2
廉价的前驱物通过二氧化硅为模板的热解合成了富含地球的过渡金属（Fe，Co或Ni）和氮掺杂的多孔碳电催化剂（MNC，其中M表示金属）。研究了材料组成和结构（即孔隙率，氮掺杂，金属同一性和氧官能化）对电化学CO 2还原反应（CO 2 RR）活性的影响。不含金属的NC表现出高的选择性，但对CO 2 RR的活性却很低。在NC材料中掺入Fe和Ni而不是Co能够显着增强活性。CO 2的一般选择性顺序相对于MNC中的金属，从水中到CO的转化为Ni> Fe≫ Co，而活性遵循Ni，Fe≫Co。值得注意的是，掺杂Ni的碳表现出高选择性，法拉第效率为一氧化碳生产的93％。Tafel分析显示，随着金属取代氮作为最活跃的位点，决定速率的步骤发生了变化。记录X射线光电子能谱和扩展的X射线吸收精细结构表明，金属原子分散在碳基质中，最有可能与四个氮原子配位，而碳原子充当第二配位壳。据推测，MNC中金属位点的第二个配位壳中的碳原子会显着影响CO 2。RR活性，因为发现碳载金属内消旋四苯基卟啉配合物的反应顺序相反。通过更好地了解CO 2 RR活性与材料结构之间的关系，可以合理地设计涉及地球富足金属的高性能多孔碳电催化剂，以进行CO 2增值。
更新日期：2018-06-12
中文翻译：
使用富含地球的金属和掺氮的碳电催化剂选择性还原水中的CO 2
廉价的前驱物通过二氧化硅为模板的热解合成了富含地球的过渡金属（Fe，Co或Ni）和氮掺杂的多孔碳电催化剂（MNC，其中M表示金属）。研究了材料组成和结构（即孔隙率，氮掺杂，金属同一性和氧官能化）对电化学CO 2还原反应（CO 2 RR）活性的影响。不含金属的NC表现出高的选择性，但对CO 2 RR的活性却很低。在NC材料中掺入Fe和Ni而不是Co能够显着增强活性。CO 2的一般选择性顺序相对于MNC中的金属，从水中到CO的转化为Ni> Fe≫ Co，而活性遵循Ni，Fe≫Co。值得注意的是，掺杂Ni的碳表现出高选择性，法拉第效率为一氧化碳生产的93％。Tafel分析显示，随着金属取代氮作为最活跃的位点，决定速率的步骤发生了变化。记录X射线光电子能谱和扩展的X射线吸收精细结构表明，金属原子分散在碳基质中，最有可能与四个氮原子配位，而碳原子充当第二配位壳。据推测，MNC中金属位点的第二个配位壳中的碳原子会显着影响CO 2。RR活性，因为发现碳载金属内消旋四苯基卟啉配合物的反应顺序相反。通过更好地了解CO 2 RR活性与材料结构之间的关系，可以合理地设计涉及地球富足金属的高性能多孔碳电催化剂，以进行CO 2增值。
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