Atomically Dispersed Alkaline‐Earth Metals as Active Centers for CO2 Electroreduction to Exclusively Produce Formate
Electrocatalytic CO2 reduction reaction (CO2RR) to produce formate (HCOOH) attracts special interest in the upgrade of waste CO2. For the selective CO2 conversion into HCOOH, the preferable binding of *OCHO compared with *COOH is a prerequisite, which presents a great challenge to the rational desig...
| Main Authors: | , , , , , |
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| Format: | Article |
| Language: | English |
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Wiley-VCH
2023-07-01
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| Series: | Small Structures |
| Subjects: | |
| Online Access: | https://doi.org/10.1002/sstr.202200358 |
| _version_ | 1827893374506500096 |
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| author | Donghai Wu Jiarui Wu Peng Lv Haobo Li Ke Chu Dongwei Ma |
| author_facet | Donghai Wu Jiarui Wu Peng Lv Haobo Li Ke Chu Dongwei Ma |
| author_sort | Donghai Wu |
| collection | DOAJ |
| description | Electrocatalytic CO2 reduction reaction (CO2RR) to produce formate (HCOOH) attracts special interest in the upgrade of waste CO2. For the selective CO2 conversion into HCOOH, the preferable binding of *OCHO compared with *COOH is a prerequisite, which presents a great challenge to the rational design of the catalytic active center. Recently, alkaline‐earth (AE) metals as active centers have been reported for electrocatalysis. Herein, the feasibility of AE metals as active centers in heterogeneous catalysis for electrocatalytic CO2RR toward HCOOH based on a series of AE metal single‐atom catalysts (SACs) is theoretically studied. High‐throughput first‐principles calculations reveal that, for all the studied systems, the AE metal active centers preferably adsorb *OCHO, enabling exclusive HCOOH production. Especially, Mg SACs embedded in graphene and Ca SAC anchored in g‐C2N can efficiently convert CO2 into HCOOH under near‐zero potential, and both systems exhibit high stability. Mechanistic investigation indicates that the AE metal active centers are highly ionic, which can strongly bind *OCHO mainly through the electrostatic attraction interaction. This study lays a theoretical foundation for the rational design of AE metal SACs for efficient CO2 electroreduction with exclusive HCOOH selectivity, and further emphasizes the potential of AE metals as active centers in heterogeneous catalysis. |
| first_indexed | 2024-03-12T21:52:17Z |
| format | Article |
| id | doaj.art-7bc48975d27046718c05b500977630a6 |
| institution | Directory Open Access Journal |
| issn | 2688-4062 |
| language | English |
| last_indexed | 2024-03-12T21:52:17Z |
| publishDate | 2023-07-01 |
| publisher | Wiley-VCH |
| record_format | Article |
| series | Small Structures |
| spelling | doaj.art-7bc48975d27046718c05b500977630a62023-07-26T01:36:01ZengWiley-VCHSmall Structures2688-40622023-07-0147n/an/a10.1002/sstr.202200358Atomically Dispersed Alkaline‐Earth Metals as Active Centers for CO2 Electroreduction to Exclusively Produce FormateDonghai Wu0Jiarui Wu1Peng Lv2Haobo Li3Ke Chu4Dongwei Ma5Key Laboratory for Special Functional Materials of Ministry of Education School of Materials Science and Engineering Henan University Kaifeng 475004 ChinaKey Laboratory for Special Functional Materials of Ministry of Education School of Materials Science and Engineering Henan University Kaifeng 475004 ChinaKey Laboratory for Special Functional Materials of Ministry of Education School of Materials Science and Engineering Henan University Kaifeng 475004 ChinaKey Laboratory for Special Functional Materials of Ministry of Education School of Materials Science and Engineering Henan University Kaifeng 475004 ChinaSchool of Materials Science and Engineering Lanzhou Jiaotong University Lanzhou 730070 ChinaKey Laboratory for Special Functional Materials of Ministry of Education School of Materials Science and Engineering Henan University Kaifeng 475004 ChinaElectrocatalytic CO2 reduction reaction (CO2RR) to produce formate (HCOOH) attracts special interest in the upgrade of waste CO2. For the selective CO2 conversion into HCOOH, the preferable binding of *OCHO compared with *COOH is a prerequisite, which presents a great challenge to the rational design of the catalytic active center. Recently, alkaline‐earth (AE) metals as active centers have been reported for electrocatalysis. Herein, the feasibility of AE metals as active centers in heterogeneous catalysis for electrocatalytic CO2RR toward HCOOH based on a series of AE metal single‐atom catalysts (SACs) is theoretically studied. High‐throughput first‐principles calculations reveal that, for all the studied systems, the AE metal active centers preferably adsorb *OCHO, enabling exclusive HCOOH production. Especially, Mg SACs embedded in graphene and Ca SAC anchored in g‐C2N can efficiently convert CO2 into HCOOH under near‐zero potential, and both systems exhibit high stability. Mechanistic investigation indicates that the AE metal active centers are highly ionic, which can strongly bind *OCHO mainly through the electrostatic attraction interaction. This study lays a theoretical foundation for the rational design of AE metal SACs for efficient CO2 electroreduction with exclusive HCOOH selectivity, and further emphasizes the potential of AE metals as active centers in heterogeneous catalysis.https://doi.org/10.1002/sstr.202200358alkaline-earth metalselectrocatalytic CO2 reduction reactionsfirst-principles calculationsformatesingle-atom catalysts |
| spellingShingle | Donghai Wu Jiarui Wu Peng Lv Haobo Li Ke Chu Dongwei Ma Atomically Dispersed Alkaline‐Earth Metals as Active Centers for CO2 Electroreduction to Exclusively Produce Formate Small Structures alkaline-earth metals electrocatalytic CO2 reduction reactions first-principles calculations formate single-atom catalysts |
| title | Atomically Dispersed Alkaline‐Earth Metals as Active Centers for CO2 Electroreduction to Exclusively Produce Formate |
| title_full | Atomically Dispersed Alkaline‐Earth Metals as Active Centers for CO2 Electroreduction to Exclusively Produce Formate |
| title_fullStr | Atomically Dispersed Alkaline‐Earth Metals as Active Centers for CO2 Electroreduction to Exclusively Produce Formate |
| title_full_unstemmed | Atomically Dispersed Alkaline‐Earth Metals as Active Centers for CO2 Electroreduction to Exclusively Produce Formate |
| title_short | Atomically Dispersed Alkaline‐Earth Metals as Active Centers for CO2 Electroreduction to Exclusively Produce Formate |
| title_sort | atomically dispersed alkaline earth metals as active centers for co2 electroreduction to exclusively produce formate |
| topic | alkaline-earth metals electrocatalytic CO2 reduction reactions first-principles calculations formate single-atom catalysts |
| url | https://doi.org/10.1002/sstr.202200358 |
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