Uncovering Atomic-Scale Stability and Reactivity in Engineered Zinc Oxide Electrocatalysts for Controllable Syngas Production

被引:66
作者
Daiyan, Rahman [1 ]
Lovell, Emma Catherine [1 ]
Huang, Bosi [2 ]
Zubair, Muhammad [1 ]
Leverett, Joshua [1 ]
Zhang, Qingran [1 ]
Lim, Sean [3 ]
Horlyck, Jonathan [1 ]
Tang, Jianbo [1 ]
Lu, Xunyu [1 ]
Kalantar-Zadeh, Kourosh [1 ]
Hart, Judy N. [2 ]
Bedford, Nicholas M. [1 ]
Amal, Rose [1 ]
机构
[1] UNSW Sydney, Sch Chem Engn, Sydney, NSW 2052, Australia
[2] UNSW Sydney, Sch Mat Sci & Engn, Sydney, NSW 2052, Australia
[3] UNSW Sydney, Elect Microscopy Unit, Sydney, NSW 2052, Australia
基金
澳大利亚研究理事会;
关键词
CO2RR flame spray pyrolysis; defective nanomaterials; syngas production; ZnO; ELECTROCHEMICAL CO2 REDUCTION; CARBON-DIOXIDE; HIGHLY EFFICIENT; OXIDATION-STATE; ELECTROREDUCTION; NANOPARTICLES; ELECTRODES; CATALYSTS; FORMATE; LIGHT;
D O I
10.1002/aenm.202001381
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 this study, scalable, flame spray synthesis is utilized to develop defective ZnO nanomaterials for the concurrent generation of H-2 and CO during electrochemical CO2 reduction reactions (CO2RR). The designed ZnO achieves an H-2/CO ratio of approximate to 1 with a large current density (j) of 40 mA cm(-2) during long-term continuous reaction at a cell voltage of 2.6 V. Through in situ atomic pair distribution function analysis, the remarkable stability of these ZnO structures is explored, addressing the knowledge gap in understanding the dynamics of oxide catalysts during CO2RR. Through optimization of synthesis conditions, ZnO facets are modulated which are shown to affect reaction selectivity, in agreement with theoretical calculations. These findings and insights on synthetic manipulation of active sites in defective metal-oxides can be used as guidelines to develop active catalysts for syngas production for renewable power-to-X to generate a range of fuels and chemicals.
引用
收藏
页数:9
相关论文
共 61 条
[1]   Photocurrent detection of chemically tuned hierarchical ZnO nanostructures grown on seed layers formed by atomic layer deposition [J].
Bang, Seokhwan ;
Lee, Seungjun ;
Ko, Youngbin ;
Park, Joohyun ;
Shin, Seokyoon ;
Seo, Hyungtak ;
Jeon, Hyeongtag .
NANOSCALE RESEARCH LETTERS, 2012, 7
[2]   RUTILE-TYPE COMPOUNDS .4. SIO2, GEO2 AND A COMPARISON WITH OTHER RUTILE-TYPE STRUCTURES [J].
BAUR, WH ;
KHAN, AA .
ACTA CRYSTALLOGRAPHICA SECTION B-STRUCTURAL CRYSTALLOGRAPHY AND CRYSTAL CHEMISTRY, 1971, B 27 (NOV15) :2133-&
[3]   Electrical properties of ZnO nanorods studied by conductive atomic force microscopy [J].
Beinik, I. ;
Kratzer, M. ;
Wachauer, A. ;
Wang, L. ;
Lechner, R. T. ;
Teichert, C. ;
Motz, C. ;
Anwand, W. ;
Brauer, G. ;
Chen, X. Y. ;
Hsu, X. Y. ;
Djurisic, A. B. .
JOURNAL OF APPLIED PHYSICS, 2011, 110 (05)
[4]   Beyond crystallography: the study of disorder, nanocrystallinity and crystallographically challenged materials with pair distribution functions [J].
Billinge, SJL ;
Kanatzidis, MG .
CHEMICAL COMMUNICATIONS, 2004, (07) :749-760
[5]   Syngas production from electrocatalytic CO2 reduction with high energetic efficiency and current density [J].
Chen, Ping ;
Jiao, Yan ;
Zhu, Yi-Han ;
Chen, Shuang-Ming ;
Song, Li ;
Jaroniec, Mietek ;
Zheng, Yao ;
Qiao, Shi-Zhang .
JOURNAL OF MATERIALS CHEMISTRY A, 2019, 7 (13) :7675-7682
[6]   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
[7]   Tunable Syngas Production through CO2 Electroreduction on Cobalt-Carbon Composite Electrocatalyst [J].
Daiyan, Rahman ;
Chen, Rui ;
Kumar, Priyank ;
Bedford, Nicholas M. ;
Qu, Jiangtao ;
Cairney, Julie M. ;
Lu, Xunyu ;
Amal, Rose .
ACS APPLIED MATERIALS & INTERFACES, 2020, 12 (08) :9307-9315
[8]   A Disquisition on the Active Sites of Heterogeneous Catalysts for Electrochemical Reduction of CO2 to Value-Added Chemicals and Fuel [J].
Daiyan, Rahman ;
Saputera, Wibawa Hendra ;
Masood, Hassan ;
Leverett, Josh ;
Lu, Xunyu ;
Amal, Rose .
ADVANCED ENERGY MATERIALS, 2020, 10 (11)
[9]   Modulating Activity through Defect Engineering of Tin Oxides for Electrochemical CO2 Reduction [J].
Daiyan, Rahman ;
Lovell, Emma Catherine ;
Bedford, Nicholas M. ;
Saputera, Wibawa Hendra ;
Wu, Kuang-Hsu ;
Lim, Sean ;
Horlyck, Jonathan ;
Ng, Yun Hau ;
Lu, Xunyu ;
Amal, Rose .
ADVANCED SCIENCE, 2019, 6 (18)
[10]   Electroreduction of CO2 to CO on a Mesoporous Carbon Catalyst with Progressively Removed Nitrogen Moieties [J].
Daiyan, Rahman ;
Tan, Xin ;
Chen, Rui ;
Saputera, Wibawa Hendra ;
Tahini, Hassan A. ;
Lovell, Emma ;
Ng, Yun Hau ;
Smith, Sean C. ;
Dai, Liming ;
Lu, Xunyu ;
Amal, Rose .
ACS ENERGY LETTERS, 2018, 3 (09) :2292-2298