Interface-Rich Highly Oxophilic Copper/Tin-Oxide Nanocomposite on Reduced Graphene Oxide for Efficient Electroreduction of CO2 to Formate

被引:17
作者
Kempasiddaiah, Manjunatha [1 ,2 ]
Samanta, Rajib [1 ,2 ]
Panigrahy, Sonali [1 ,2 ]
Barman, Sudip [1 ,2 ]
机构
[1] HBNI, Natl Inst Sci Educ & Res NISER, Sch Chem Sci, Bhubaneswar 752050, Orissa, India
[2] Homi Bhabha Natl Inst, Mumbai 400094, Maharashtra, India
关键词
Reduced graphene oxide; Nanocomposites; Electrochemical CO2 reduction; Interfaces; Oxophilicity; Formate; ELECTROCHEMICAL REDUCTION; CARBON-DIOXIDE; BIMETALLIC CATALYSTS; TIN ELECTRODES; FORMIC-ACID; SELECTIVITY; CU; SURFACE; NANOPARTICLES; WATER;
D O I
10.1021/acsaem.2c04130
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
In recent days, it has been reported that bimetallic electrocatalysts can increase the activity for electrochemical formate (HCOO-) production during CO2 reduction. However, they still have some apparent drawbacks such as poor selectivity and durability. In the current work, notable improvements in the electrochemical CO2 reduction (CO2RR) to formate production were accomplished by incorporation of reduced graphene oxide (rGO) into nanostructured bimetallic CuSnOx electrocatalysts (CuxSnOx/rGO). The interface-rich mixed crystalline-amorphous nanostructured Cu0.33SnOx/rGO nanocomposite is able to enhance the electrocatalytical activity, resulting in conversion of CO2 to formate with lower overpotential of 590 mV vs RHE. The control experiments show that the presence of SnOx in the catalyst considerably increased electrocatalytic activity and product selectivity toward formate production. Further, the increased oxophilicity of the Cu0.33SnOx/rGO nanocomposite supports the plausible CO2 reduction mechanism through the formation of bicarbonate intermediate, as demonstrated by CO stripping studies. The Cu0.33SnOx/rGO had maximum formate faradaic efficiency (80.62%) at lower potential of -0.69 V (RHE), which is 2.09 and 1.85 times better than those of CuSnOx/rGO and Cu3SnOx/rGO nanocomposites, respectively. The catalytic performance may be attributed to synergistic interaction, the presence of interfaces, higher electrochemical surface area, and the mixed crystalline-amorphous nature of Cu0.33SnOx/rGO nanocomposite. Thus, the obtained results gave rise to a practical method for boosting the activity and product selectivity of electrocatalysts for efficient CO2 conversion.
引用
收藏
页码:3020 / 3031
页数:12
相关论文
共 70 条
[1]   Copper nanoparticles stabilized by reduced graphene oxide for CO2 reduction reaction [J].
Alves D.C.B. ;
Silva R. ;
Voiry D. ;
Asefa T. ;
Chhowalla M. .
Materials for Renewable and Sustainable Energy, 2015, 4 (01)
[2]   Electrodeposition of Tin-Based Electrocatalysts with Different Surface Tin Species Distributions for Electrochemical Reduction of CO2 to HCOOH [J].
An, Xiaowei ;
Li, Shasha ;
Yoshida, Akihiro ;
Wang, Zhongde ;
Hao, Xiaogang ;
Abudula, Abuliti ;
Guan, Guoqing .
ACS SUSTAINABLE CHEMISTRY & ENGINEERING, 2019, 7 (10) :9360-9368
[3]  
Baddour F. G., 2020, J AM CHEM SOC
[4]   Mechanistic Insights into the Reduction of CO2 on Tin Electrodes using in Situ ATR-IR Spectroscopy [J].
Baruch, Maor F. ;
Pander, James E., III ;
White, James L. ;
Bocarsly, Andrew B. .
ACS CATALYSIS, 2015, 5 (05) :3148-3156
[5]   Study of Reduced Graphene Oxide Preparation by Hummers' Method and Related Characterization [J].
Cao, Ning ;
Zhang, Yuan .
JOURNAL OF NANOMATERIALS, 2015, 2015
[6]   Palladium nanoparticles supported on amine-functionalized SiO2 for the catalytic hexavalent chromium reduction [J].
Celebi, Metin ;
Yurderi, Mehmet ;
Bulut, Ahrnet ;
Kaya, Murat ;
Zahmakiran, Mehmet .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2016, 180 :53-64
[7]   Modulating charge separation via in situ hydrothermal assembly of low content Bi2S3 into UiO-66 for efficient photothermocatalytic CO2 reduction [J].
Chen, Xi ;
Li, Qiang ;
Li, Juanjuan ;
Chen, Jing ;
Jia, Hongpeng .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2020, 270
[8]   Aqueous CO2 Reduction at Very Low Overpotential on Oxide-Derived Au Nanoparticles [J].
Chen, Yihong ;
Li, Christina W. ;
Kanan, Matthew W. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2012, 134 (49) :19969-19972
[9]   Tin Oxide Dependence of the CO2 Reduction Efficiency on Tin Electrodes and Enhanced Activity for Tin/Tin Oxide Thin-Film Catalysts [J].
Chen, Yihong ;
Kanan, Matthew W. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2012, 134 (04) :1986-1989
[10]   Electroreduction of Carbon Dioxide on Copper-Based Electrodes: Activity of Copper Single Crystals and Copper-Gold Alloys [J].
Christophe, J. ;
Doneux, Th. ;
Buess-Herman, C. .
ELECTROCATALYSIS, 2012, 3 (02) :139-146