Mechanistic insights into the effect of halide anions on electroreduction pathways of CO 2 to C 1 product at Cu/H 2 O electrochemical interfaces
Various elementary reaction steps during CO 2 electroreduction into C 1 product are systematically studied at specifically adsorbed halide anions modified Cu(111)/H 2 O interfaces via theoretical calculations with the aim of identifying the effect of halide anions X − (X = F, Cl, Br, I) on CO 2 elec...
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| Veröffentlicht in: | Catalysis science & technology 2023-12, Vol.13 (24), p.7149-7161 |
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| creator | Ou, Lihui You, Wanli Jin, Junling |
| description | Various elementary reaction steps during CO
2
electroreduction into C
1
product are systematically studied at specifically adsorbed halide anions modified Cu(111)/H
2
O interfaces
via
theoretical calculations with the aim of identifying the effect of halide anions X
−
(X = F, Cl, Br, I) on CO
2
electroreduction reaction activity, mechanisms and product selectivity in this work. Our present studies show that halogen atoms can be adsorbed on the Cu electrodes during CO
2
electroreduction, thus leading to notable electronic interactions between halogen atoms and Cu(111)/H
2
O interface. It is found that halogen atoms can gain electrons in the order of F > Cl > Br > I, showing that the adsorbed halide anions can be formed. The presence of halide anions can notably be favor of CO formations. CO electroreduction pathways towards C
1
product at Br
−
and I
−
modified Cu(111)/H
2
O interfaces are examined due to poor selectivity of CO electroreduction into CHO at F
−
and Cl
−
modified Cu(111)/H
2
O interfaces. The calculated results indicate that the presence of Br
−
and I
−
facilitate CO
2
electroreduction into C
1
product since notably enhanced CO
2
electroreduction activity can be achieved, which may be ascribed to the formations of chemically adsorbed anion radical ˙CO
2
−
and more positive onset potentials for CO formations. Notably, it is found that the electroreduction pathways of CO
2
into CH
4
and CH
3
OH product may be able to parallelly occur at Br
−
and I
−
modified Cu(111)/H
2
O interfaces, whereas only CH
4
production pathways can occur at clean Cu(111)/H
2
O interface. Thus, it can be concluded that the presence of halogen anions on Cu alter mechanism and product selectivity of CO
2
electroreduction. Our present mechanistic insights into this effect may be able to give a theoretical guideline for control of mechanisms and product selectivity during CO
2
electroreduction. |
| doi_str_mv | 10.1039/D3CY01338C |
| format | Article |
| fullrecord | <record><control><sourceid>crossref</sourceid><recordid>TN_cdi_crossref_primary_10_1039_D3CY01338C</recordid><sourceformat>XML</sourceformat><sourcesystem>PC</sourcesystem><sourcerecordid>10_1039_D3CY01338C</sourcerecordid><originalsourceid>FETCH-LOGICAL-c76C-46ab77b07919ddc866d9c708d2d5222a6550e363f7e800ef50c573cbb76de4cc3</originalsourceid><addsrcrecordid>eNpFUMtqwzAQFKWFhjSXfsGeC24ky5bsY1EfKaT4kktPRpZWtYtjB0mh5C_6ybXpay877MzOwBByzegto7xc33P1ShnnhToji5RmWZJJwc7_cM4vySqEdzpNVjJapAvy-YKm1UMXYmegG0L31sYwgThCbBHQOTQRRget7juLMEnHIcA4APYT40eP9mjidISDju2HPoVZrSpIYfJQwODgx1kCOoI6rjcTUf0-mxb3ndH9HIjeaYPhilw43Qdc_ewl2T0-7NQm2VZPz-pumxgpVJIJ3UjZUFmy0lpTCGFLI2lhU5unaapFnlPkgjuJBaXocmpyyU3TSGExM4Yvyc23rfFjCB5dffDdXvtTzWg9t1n_t8m_AMU1Z_o</addsrcrecordid><sourcetype>Aggregation Database</sourcetype><iscdi>true</iscdi><recordtype>article</recordtype></control><display><type>article</type><title>Mechanistic insights into the effect of halide anions on electroreduction pathways of CO 2 to C 1 product at Cu/H 2 O electrochemical interfaces</title><source>Royal Society Of Chemistry Journals 2008-</source><creator>Ou, Lihui ; You, Wanli ; Jin, Junling</creator><creatorcontrib>Ou, Lihui ; You, Wanli ; Jin, Junling</creatorcontrib><description>Various elementary reaction steps during CO
2
electroreduction into C
1
product are systematically studied at specifically adsorbed halide anions modified Cu(111)/H
2
O interfaces
via
theoretical calculations with the aim of identifying the effect of halide anions X
−
(X = F, Cl, Br, I) on CO
2
electroreduction reaction activity, mechanisms and product selectivity in this work. Our present studies show that halogen atoms can be adsorbed on the Cu electrodes during CO
2
electroreduction, thus leading to notable electronic interactions between halogen atoms and Cu(111)/H
2
O interface. It is found that halogen atoms can gain electrons in the order of F > Cl > Br > I, showing that the adsorbed halide anions can be formed. The presence of halide anions can notably be favor of CO formations. CO electroreduction pathways towards C
1
product at Br
−
and I
−
modified Cu(111)/H
2
O interfaces are examined due to poor selectivity of CO electroreduction into CHO at F
−
and Cl
−
modified Cu(111)/H
2
O interfaces. The calculated results indicate that the presence of Br
−
and I
−
facilitate CO
2
electroreduction into C
1
product since notably enhanced CO
2
electroreduction activity can be achieved, which may be ascribed to the formations of chemically adsorbed anion radical ˙CO
2
−
and more positive onset potentials for CO formations. Notably, it is found that the electroreduction pathways of CO
2
into CH
4
and CH
3
OH product may be able to parallelly occur at Br
−
and I
−
modified Cu(111)/H
2
O interfaces, whereas only CH
4
production pathways can occur at clean Cu(111)/H
2
O interface. Thus, it can be concluded that the presence of halogen anions on Cu alter mechanism and product selectivity of CO
2
electroreduction. Our present mechanistic insights into this effect may be able to give a theoretical guideline for control of mechanisms and product selectivity during CO
2
electroreduction.</description><identifier>ISSN: 2044-4753</identifier><identifier>EISSN: 2044-4761</identifier><identifier>DOI: 10.1039/D3CY01338C</identifier><language>eng</language><ispartof>Catalysis science & technology, 2023-12, Vol.13 (24), p.7149-7161</ispartof><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c76C-46ab77b07919ddc866d9c708d2d5222a6550e363f7e800ef50c573cbb76de4cc3</citedby><cites>FETCH-LOGICAL-c76C-46ab77b07919ddc866d9c708d2d5222a6550e363f7e800ef50c573cbb76de4cc3</cites><orcidid>0000-0001-5177-2404</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>314,780,784,27924,27925</link.rule.ids></links><search><creatorcontrib>Ou, Lihui</creatorcontrib><creatorcontrib>You, Wanli</creatorcontrib><creatorcontrib>Jin, Junling</creatorcontrib><title>Mechanistic insights into the effect of halide anions on electroreduction pathways of CO 2 to C 1 product at Cu/H 2 O electrochemical interfaces</title><title>Catalysis science & technology</title><description>Various elementary reaction steps during CO
2
electroreduction into C
1
product are systematically studied at specifically adsorbed halide anions modified Cu(111)/H
2
O interfaces
via
theoretical calculations with the aim of identifying the effect of halide anions X
−
(X = F, Cl, Br, I) on CO
2
electroreduction reaction activity, mechanisms and product selectivity in this work. Our present studies show that halogen atoms can be adsorbed on the Cu electrodes during CO
2
electroreduction, thus leading to notable electronic interactions between halogen atoms and Cu(111)/H
2
O interface. It is found that halogen atoms can gain electrons in the order of F > Cl > Br > I, showing that the adsorbed halide anions can be formed. The presence of halide anions can notably be favor of CO formations. CO electroreduction pathways towards C
1
product at Br
−
and I
−
modified Cu(111)/H
2
O interfaces are examined due to poor selectivity of CO electroreduction into CHO at F
−
and Cl
−
modified Cu(111)/H
2
O interfaces. The calculated results indicate that the presence of Br
−
and I
−
facilitate CO
2
electroreduction into C
1
product since notably enhanced CO
2
electroreduction activity can be achieved, which may be ascribed to the formations of chemically adsorbed anion radical ˙CO
2
−
and more positive onset potentials for CO formations. Notably, it is found that the electroreduction pathways of CO
2
into CH
4
and CH
3
OH product may be able to parallelly occur at Br
−
and I
−
modified Cu(111)/H
2
O interfaces, whereas only CH
4
production pathways can occur at clean Cu(111)/H
2
O interface. Thus, it can be concluded that the presence of halogen anions on Cu alter mechanism and product selectivity of CO
2
electroreduction. Our present mechanistic insights into this effect may be able to give a theoretical guideline for control of mechanisms and product selectivity during CO
2
electroreduction.</description><issn>2044-4753</issn><issn>2044-4761</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2023</creationdate><recordtype>article</recordtype><recordid>eNpFUMtqwzAQFKWFhjSXfsGeC24ky5bsY1EfKaT4kktPRpZWtYtjB0mh5C_6ybXpay877MzOwBByzegto7xc33P1ShnnhToji5RmWZJJwc7_cM4vySqEdzpNVjJapAvy-YKm1UMXYmegG0L31sYwgThCbBHQOTQRRget7juLMEnHIcA4APYT40eP9mjidISDju2HPoVZrSpIYfJQwODgx1kCOoI6rjcTUf0-mxb3ndH9HIjeaYPhilw43Qdc_ewl2T0-7NQm2VZPz-pumxgpVJIJ3UjZUFmy0lpTCGFLI2lhU5unaapFnlPkgjuJBaXocmpyyU3TSGExM4Yvyc23rfFjCB5dffDdXvtTzWg9t1n_t8m_AMU1Z_o</recordid><startdate>20231211</startdate><enddate>20231211</enddate><creator>Ou, Lihui</creator><creator>You, Wanli</creator><creator>Jin, Junling</creator><scope>AAYXX</scope><scope>CITATION</scope><orcidid>https://orcid.org/0000-0001-5177-2404</orcidid></search><sort><creationdate>20231211</creationdate><title>Mechanistic insights into the effect of halide anions on electroreduction pathways of CO 2 to C 1 product at Cu/H 2 O electrochemical interfaces</title><author>Ou, Lihui ; You, Wanli ; Jin, Junling</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c76C-46ab77b07919ddc866d9c708d2d5222a6550e363f7e800ef50c573cbb76de4cc3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2023</creationdate><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Ou, Lihui</creatorcontrib><creatorcontrib>You, Wanli</creatorcontrib><creatorcontrib>Jin, Junling</creatorcontrib><collection>CrossRef</collection><jtitle>Catalysis science & technology</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Ou, Lihui</au><au>You, Wanli</au><au>Jin, Junling</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Mechanistic insights into the effect of halide anions on electroreduction pathways of CO 2 to C 1 product at Cu/H 2 O electrochemical interfaces</atitle><jtitle>Catalysis science & technology</jtitle><date>2023-12-11</date><risdate>2023</risdate><volume>13</volume><issue>24</issue><spage>7149</spage><epage>7161</epage><pages>7149-7161</pages><issn>2044-4753</issn><eissn>2044-4761</eissn><abstract>Various elementary reaction steps during CO
2
electroreduction into C
1
product are systematically studied at specifically adsorbed halide anions modified Cu(111)/H
2
O interfaces
via
theoretical calculations with the aim of identifying the effect of halide anions X
−
(X = F, Cl, Br, I) on CO
2
electroreduction reaction activity, mechanisms and product selectivity in this work. Our present studies show that halogen atoms can be adsorbed on the Cu electrodes during CO
2
electroreduction, thus leading to notable electronic interactions between halogen atoms and Cu(111)/H
2
O interface. It is found that halogen atoms can gain electrons in the order of F > Cl > Br > I, showing that the adsorbed halide anions can be formed. The presence of halide anions can notably be favor of CO formations. CO electroreduction pathways towards C
1
product at Br
−
and I
−
modified Cu(111)/H
2
O interfaces are examined due to poor selectivity of CO electroreduction into CHO at F
−
and Cl
−
modified Cu(111)/H
2
O interfaces. The calculated results indicate that the presence of Br
−
and I
−
facilitate CO
2
electroreduction into C
1
product since notably enhanced CO
2
electroreduction activity can be achieved, which may be ascribed to the formations of chemically adsorbed anion radical ˙CO
2
−
and more positive onset potentials for CO formations. Notably, it is found that the electroreduction pathways of CO
2
into CH
4
and CH
3
OH product may be able to parallelly occur at Br
−
and I
−
modified Cu(111)/H
2
O interfaces, whereas only CH
4
production pathways can occur at clean Cu(111)/H
2
O interface. Thus, it can be concluded that the presence of halogen anions on Cu alter mechanism and product selectivity of CO
2
electroreduction. Our present mechanistic insights into this effect may be able to give a theoretical guideline for control of mechanisms and product selectivity during CO
2
electroreduction.</abstract><doi>10.1039/D3CY01338C</doi><tpages>13</tpages><orcidid>https://orcid.org/0000-0001-5177-2404</orcidid></addata></record> |
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| ispartof | Catalysis science & technology, 2023-12, Vol.13 (24), p.7149-7161 |
| issn | 2044-4753 2044-4761 |
| language | eng |
| recordid | cdi_crossref_primary_10_1039_D3CY01338C |
| source | Royal Society Of Chemistry Journals 2008- |
| title | Mechanistic insights into the effect of halide anions on electroreduction pathways of CO 2 to C 1 product at Cu/H 2 O electrochemical interfaces |
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