水系体系中CO_2在稀土(Nd)(Ⅲ)双酞菁修饰电极上的电催化还原研究
|
摘要
探讨了CO_2在稀土(Nd)(Ⅲ)双酞菁修饰电极上的电催还原行为。通过滴涂法将稀土(Nd)(Ⅲ)双酞菁担载在玻碳电极上制备成它的修饰电极,在水溶液中利用循环伏安、红外光谱法等方法研究制备的修饰电极对CO_2的电催化还原性能。结果表明,所制备的稀土(Nd)(Ⅲ)双酞菁修饰电极对CO_2的电催化还原有较高的活性,还原电流随修饰量增加而变大,修饰电极的还原电流与溶液的pH值有关,随着pH值变大,还原峰向负方向移动。实验结果表明,稀土(Nd)(Ⅲ)双酞菁修饰电极对二氧化碳电化学还原具有很好的电催化活性,在该修饰电极上,CO_2可在较正的电位下被还原。
The aim of this study was to investigate the electrocatalytic reduction of CO_2 at rare earth(Nd)(Ⅲ)diphthalocyanine modified electrodes.Rare earth(Nd)(Ⅲ)diphthalocyanine was loaded on glassy carbon electrode by dropping coating method to prepare its modified electrode.The electrocatalytic reduction performance of the modified electrode for CO_2 was studied by cyclic voltammetry and infrared spectroscopy in aqueous solution.The results show that the rare earth(Nd)(Ⅲ)diphthalocyanine modified electrode prepared in this study has high activity for the electrocatalytic reduction of CO_2.The reduction current increases with the increase of the modification amount.The reduction current of the modified electrode is related to the pH value of the solution.As the pH value increases,the reduction peak moves to the negative direction.The experimental results show that the rare earth(Nd)(Ⅲ)diphthalocyanine modified electrode has good electrocatalytic activity for the electrochemical reduction of carbon dioxide.On the modified electrode,CO_2 can be reduced at a relative positive potential.
The aim of this study was to investigate the electrocatalytic reduction of CO_2 at rare earth(Nd)(Ⅲ)diphthalocyanine modified electrodes.Rare earth(Nd)(Ⅲ)diphthalocyanine was loaded on glassy carbon electrode by dropping coating method to prepare its modified electrode.The electrocatalytic reduction performance of the modified electrode for CO_2 was studied by cyclic voltammetry and infrared spectroscopy in aqueous solution.The results show that the rare earth(Nd)(Ⅲ)diphthalocyanine modified electrode prepared in this study has high activity for the electrocatalytic reduction of CO_2.The reduction current increases with the increase of the modification amount.The reduction current of the modified electrode is related to the pH value of the solution.As the pH value increases,the reduction peak moves to the negative direction.The experimental results show that the rare earth(Nd)(Ⅲ)diphthalocyanine modified electrode has good electrocatalytic activity for the electrochemical reduction of carbon dioxide.On the modified electrode,CO_2 can be reduced at a relative positive potential.
引文
[1]白晓芳,陈为,王白银,等.二氧化碳电化学还原的研究进展[J].物理化学学报(Acta Phys.-Chim.Sin.),2017,33(12):2388-2403.
[2]HORI Y,MURATA A,KIKUCHI K,et al.Atomic arrangement dependence of reduction rates of carbon dioxide on iridium single crastal electrodes[J].Journal of Electroanalytical Chemistry,1995,381:261-264.
[3]KOLELI F,ATILAN T,PALAMUT N.Electrochemical reduction of CO2at Pb and Sn electrodes in a fixed-bed reactor in aqueous K2CO3and KHCO3media[J].Journal of Applied Electrochemistry,2003,33(5):447-450.
[4]CHRISTOPHE J,DONEUX T H,BUESS-HERMAN C,Electroreduction of carbon dioxide on copper-based electrodes:activity of copper single crystals and copper-gold alloys[J].Electrocatalysis,2012,3(2):139-146.
[5]SUBRAMANIAN K,ASOKAN K,JEEVARATHINAM D,et al.Electrochemical membrane reactor for the reduction of carbondioxide to formate[J].Journal of Applied Electrochemistry,2007,37(2):255-260.
[6]谭幸楠,金葆康.Au25/L-半胱氨酸修饰金电极上CO2的电化学还原[J].安徽大学学报(Journal of Anhui Agricultural University),2018,42(3):71-78.
[7]秦军荣.基于金属纳米粒子修饰电极在吡啶水溶液中电催化还原CO2的研究[D].上海:上海师范大学,2015.
[8]杨刚,余志鹏,张杰,等.高效二氧化碳电催化还原反应花状钴催化剂的制备及性能[J].催化学报(Chinese Journal of Catalysis),2018,39:914-919.
[9]COLLIN J P,SAUVAGE J.Electrochemical reduction of carbon dioxide mediated by molecular catalysts[J].Coord.Chem.Rev.,1989,93,245-268.
[10]HAN Na,WANG Yu,MA Lu.Supported cobalt polyphthalocyanine for high-performance electrocatalytic CO2reduction[J].Chem.,2017,3(4):652-664.
[11]张英菊,梁斌,潘玉珍,等.四叔丁基金属酞菁催化活化CO2与环氧丙烷的环加成反应[J].催化学报(Chinese Journal of Catalysis),2003,24(10):765-768.
[12]李军,崔凤霞,李荣.二氧化碳还原技术研究进展[J].精细石油化工(Speciality Petrochemicals),2017,34(2):75-82.
[13]谭幸楠.修饰金电极界面上CO2的电化学还原研究[D].合肥:安徽大学,2017.
[14]KRAMER ORCID W W,MCCRORY C C L.Polymer coordination promotes selective CO2 reduction by cobalt phthalocyanine[J].Chem.Sci.,2016(7):2506-2515.
[2]HORI Y,MURATA A,KIKUCHI K,et al.Atomic arrangement dependence of reduction rates of carbon dioxide on iridium single crastal electrodes[J].Journal of Electroanalytical Chemistry,1995,381:261-264.
[3]KOLELI F,ATILAN T,PALAMUT N.Electrochemical reduction of CO2at Pb and Sn electrodes in a fixed-bed reactor in aqueous K2CO3and KHCO3media[J].Journal of Applied Electrochemistry,2003,33(5):447-450.
[4]CHRISTOPHE J,DONEUX T H,BUESS-HERMAN C,Electroreduction of carbon dioxide on copper-based electrodes:activity of copper single crystals and copper-gold alloys[J].Electrocatalysis,2012,3(2):139-146.
[5]SUBRAMANIAN K,ASOKAN K,JEEVARATHINAM D,et al.Electrochemical membrane reactor for the reduction of carbondioxide to formate[J].Journal of Applied Electrochemistry,2007,37(2):255-260.
[6]谭幸楠,金葆康.Au25/L-半胱氨酸修饰金电极上CO2的电化学还原[J].安徽大学学报(Journal of Anhui Agricultural University),2018,42(3):71-78.
[7]秦军荣.基于金属纳米粒子修饰电极在吡啶水溶液中电催化还原CO2的研究[D].上海:上海师范大学,2015.
[8]杨刚,余志鹏,张杰,等.高效二氧化碳电催化还原反应花状钴催化剂的制备及性能[J].催化学报(Chinese Journal of Catalysis),2018,39:914-919.
[9]COLLIN J P,SAUVAGE J.Electrochemical reduction of carbon dioxide mediated by molecular catalysts[J].Coord.Chem.Rev.,1989,93,245-268.
[10]HAN Na,WANG Yu,MA Lu.Supported cobalt polyphthalocyanine for high-performance electrocatalytic CO2reduction[J].Chem.,2017,3(4):652-664.
[11]张英菊,梁斌,潘玉珍,等.四叔丁基金属酞菁催化活化CO2与环氧丙烷的环加成反应[J].催化学报(Chinese Journal of Catalysis),2003,24(10):765-768.
[12]李军,崔凤霞,李荣.二氧化碳还原技术研究进展[J].精细石油化工(Speciality Petrochemicals),2017,34(2):75-82.
[13]谭幸楠.修饰金电极界面上CO2的电化学还原研究[D].合肥:安徽大学,2017.
[14]KRAMER ORCID W W,MCCRORY C C L.Polymer coordination promotes selective CO2 reduction by cobalt phthalocyanine[J].Chem.Sci.,2016(7):2506-2515.