journal article·2022-07-20Open access

Engineering the Interfacial Microenvironment via Surface Hydroxylation to Realize the Global Optimization of Electrochemical CO2 Reduction

Xu Han, Ting Zhang, Martí Biset-Peiró, Xuan Zhang, Jian Li, Weiqiang Tang, Pengyi Tang, Joan Ramon Morante, Jordi Arbiol

ACS Applied Materials & Interfaces· Volume 14· Issue 28

Abstract

The adsorption and activation of CO 2 on the electrode interface is a prerequisite and key step for electrocatalytic CO 2 reduction reaction (eCO 2 RR). Regulating the interfacial microenvironment to promote the adsorption and activation of CO 2 is thus of great significance to optimize overall conversion efficiency. Herein, a CO 2philic hydroxyl coordinated ZnO (ZnO-OH) catalyst is fabricated, for the first time, via a facile MOF-assisted method. In comparison to the commercial ZnO, the as-prepared ZnO-OH exhibits much higher selectivity toward CO at lower applied potential, reaching a Faradaic efficiency of 85% at -0.95 V versus RHE. To the best of our knowledge, such selectivity is one of the best records in ZnO-based catalysts reported till date. Density functional theory calculations reveal that the coordinated surficial -OH groups are not only favorable to interact with CO 2 molecules but also function in synergy to decrease the energy barrier of the rate-determining step and maintain a higher charge density of potential active sites as well as inhibit undesired hydrogen evolution reaction. Our results indicate that engineering the interfacial microenvironment through the introduction of CO 2 -philic groups is a promising way to achieve the global optimization of eCO 2 RR via promoting adsorption and activation of CO 2 .
Source: openalex_inverted_index · Quality: baseline

Research context

OpenAlex topics: CO2 Reduction Techniques and Catalysts · Ionic liquids properties and applications · Advanced battery technologies research

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Catalan Institute of Nanoscience and Nanotechnology (ICN2), CSIC and BIST, Campus UAB, Bellaterra, Barcelona, 08193 Catalonia, Spain

Catalonia Institute for Energy Research (IREC), Jardins de les Dones de Negre 1, Sant Adrià del Besòs,Barcelona, 08930 Catalonia, Spain

Department of Materials Engineering, KU Leuven, 3001 Leuven, Belgium

Laboratory of Renewable Energy Science and Engineering, Institute of Mechanical Engineering EPFL, Station 9, 1015 Lausanne, Switzerland

State Key Laboratory of Chemical Engineering and School of Chemical Engineering, East China University of Science and Technology, 200237 Shanghai, China

State Key Laboratory of Information Functional Materials, 2020 X-Lab, Shanghai Institute of Microsystem and Information Technology, Chinese Academy of Sciences, 200050 Shanghai, China

Department of Physics, Universitat de Barcelona, Barcelona, 08028 Catalonia, Spain

ICREA, Pg. Lluís Companys 23, Barcelona, 08010 Catalonia, Spain

Funding

Ministerio de Ciencia, Innovaci?n y Universidades · Agencia Estatal de Investigaci?n · Ministerio de Econom?a y Competitividad · Fonds Wetenschappelijk Onderzoek · Generalitat de Catalunya · China Scholarship Council · CERCA Programme

References (56)

Show source-provided references
1. 10.1002/anie.20210181810.1002/anie.202101818 ↗
2. 10.1038/s41586-020-2242-810.1038/s41586-020-2242-8 ↗
3. 10.1021/jacs.1c1125310.1021/jacs.1c11253 ↗
4. 10.1016/s1872-2067(21)63866-410.1016/s1872-2067(21)63866-4 ↗
5. 10.1016/j.chempr.2019.06.01910.1016/j.chempr.2019.06.019 ↗
6. 10.1021/acsami.0c1903110.1021/acsami.0c19031 ↗
7. 10.1021/cr050199410.1021/cr0501994 ↗
8. 10.1126/science.120978610.1126/science.1209786 ↗
9. 10.1002/adma.20150476610.1002/adma.201504766 ↗
10. 10.1002/advs.20170027510.1002/advs.201700275 ↗
11. 10.1016/j.matt.2019.07.00310.1016/j.matt.2019.07.003 ↗
12. 10.1016/j.jechem.2021.08.06010.1016/j.jechem.2021.08.060 ↗
13. 10.1021/acs.chemrev.8b0048110.1021/acs.chemrev.8b00481 ↗
14. 10.1021/acscatal.0c0471410.1021/acscatal.0c04714 ↗
15. 10.1021/acssuschemeng.0c0348110.1021/acssuschemeng.0c03481 ↗
16. 10.1021/acssuschemeng.7b0246010.1021/acssuschemeng.7b02460 ↗
17. 10.1021/acsami.0c2030210.1021/acsami.0c20302 ↗
18. 10.1002/anie.20171125510.1002/anie.201711255 ↗
19. 10.1002/aenm.20200138110.1002/aenm.202001381 ↗
20. 10.1039/d0cs00835d10.1039/d0cs00835d ↗
21. 10.1039/c1nr11114k10.1039/c1nr11114k ↗
22. 10.1021/jacs.7b0676510.1021/jacs.7b06765 ↗
23. 10.1002/celc.20170131610.1002/celc.201701316 ↗
24. 10.1093/nsr/nwy05110.1093/nsr/nwy051 ↗
25. 10.1002/anie.20210932910.1002/anie.202109329 ↗
26. 10.1021/jacs.8b1378610.1021/jacs.8b13786 ↗
27. 10.1002/anie.20180146310.1002/anie.201801463 ↗
28. 10.1016/j.chempr.2018.01.01910.1016/j.chempr.2018.01.019 ↗
29. 10.1016/j.jcat.2015.12.00110.1016/j.jcat.2015.12.001 ↗
30. 10.1002/anie.20210474710.1002/anie.202104747 ↗
31. 10.1002/anie.20181471110.1002/anie.201814711 ↗
32. 10.1021/acsami.6b1218910.1021/acsami.6b12189 ↗
33. 10.1002/adfm.20211144610.1002/adfm.202111446 ↗
34. 10.1021/jacs.7b1158910.1021/jacs.7b11589 ↗
35. 10.1021/ic801865w10.1021/ic801865w ↗
36. 10.1021/acs.inorgchem.8b0124210.1021/acs.inorgchem.8b01242 ↗
37. 10.1021/nl300554t10.1021/nl300554t ↗
38. 10.1021/nl300840q10.1021/nl300840q ↗
39. 10.1021/acs.nanolett.9b0045910.1021/acs.nanolett.9b00459 ↗
40. 10.1002/adfm.20210099410.1002/adfm.202100994 ↗
41. 10.1021/ja501866r10.1021/ja501866r ↗
42. 10.1186/1556-276x-7-29010.1186/1556-276x-7-290 ↗
43. 10.1002/solr.20180008610.1002/solr.201800086 ↗
44. 10.1021/acsomega.7b0142010.1021/acsomega.7b01420 ↗
45. 10.1021/jp810680910.1021/jp8106809 ↗
46. 10.1002/anie.20191199510.1002/anie.201911995 ↗
47. 10.1039/d1ee01592c10.1039/d1ee01592c ↗
48. 10.1021/acsnano.9b0852810.1021/acsnano.9b08528 ↗
49. 10.1039/c2cc16961d10.1039/c2cc16961d ↗
50. 10.1021/acscatal.8b0218110.1021/acscatal.8b02181 ↗
51. 10.1016/j.joule.2018.11.00810.1016/j.joule.2018.11.008 ↗
52. 10.1021/ja301097810.1021/ja3010978 ↗
53. 10.1126/science.aaw751510.1126/science.aaw7515 ↗
54. 10.1016/j.apcatb.2022.12109310.1016/j.apcatb.2022.121093 ↗
55. 10.1016/s1872-2067(20)63754-810.1016/s1872-2067(20)63754-8 ↗
56. 10.1016/j.apcatb.2020.11906010.1016/j.apcatb.2020.119060 ↗