{"id":2948,"date":"2023-02-17T10:59:00","date_gmt":"2023-02-17T09:59:00","guid":{"rendered":"https:\/\/site.uit.no\/nordco2\/?p=2948"},"modified":"2024-10-11T12:20:38","modified_gmt":"2024-10-11T10:20:38","slug":"research-article-au-and-uio","status":"publish","type":"post","link":"https:\/\/site.uit.no\/nordco2\/2023\/02\/17\/research-article-au-and-uio\/","title":{"rendered":"Research Article: AU and UiO"},"content":{"rendered":"\n<figure class=\"wp-block-image size-full\"><img fetchpriority=\"high\" decoding=\"async\" width=\"972\" height=\"526\" src=\"https:\/\/site.uit.no\/nordco2\/wp-content\/uploads\/sites\/344\/2024\/01\/images_large_ja2c06454_0016-2.jpeg\" alt=\"graphical abstract\" class=\"wp-image-2949\" srcset=\"https:\/\/site.uit.no\/nordco2\/wp-content\/uploads\/sites\/344\/2024\/01\/images_large_ja2c06454_0016-2.jpeg 972w, https:\/\/site.uit.no\/nordco2\/wp-content\/uploads\/sites\/344\/2024\/01\/images_large_ja2c06454_0016-2-300x162.jpeg 300w, https:\/\/site.uit.no\/nordco2\/wp-content\/uploads\/sites\/344\/2024\/01\/images_large_ja2c06454_0016-2-768x416.jpeg 768w, https:\/\/site.uit.no\/nordco2\/wp-content\/uploads\/sites\/344\/2024\/01\/images_large_ja2c06454_0016-2-693x375.jpeg 693w\" sizes=\"(max-width: 972px) 100vw, 972px\" \/><\/figure>\n\n\n\n<p><strong>Title:<\/strong><br><a href=\"https:\/\/pubs.acs.org\/doi\/10.1021\/acscatal.2c05951\" data-type=\"URL\" data-id=\"https:\/\/pubs.acs.org\/doi\/10.1021\/acscatal.2c05951\">Exploring the Parameters Controlling Product Selectivity in Electrochemical CO<sub>2<\/sub>\u00a0Reduction in Competition with Hydrogen Evolution Employing Manganese Bipyridine Complexes<\/a><\/p>\n\n\n\n<p><strong>Abstract:<\/strong><br>Selective reduction of CO<sub>2<\/sub>\u00a0is an efficient solution for producing nonfossil-based chemical feedstocks and simultaneously alleviating the increasing atmospheric concentration of this greenhouse gas. With this aim, molecular electrocatalysts are being extensively studied, although selectivity remains an issue. In this work, a combined experimental\u2013computational study explores how the molecular structure of Mn-based complexes determines the dominant product in the reduction of CO<sub>2<\/sub>\u00a0to HCOOH, CO, and H<sub>2<\/sub>. In contrast to previous Mn(bpy-R)(CO)<sub>3<\/sub>Br catalysts containing alkyl amines in the vicinity of the Br ligand, here, we report that bpy-based macrocycles locking these amines at the side opposite to the Br ligand change the product selectivity from HCOOH to H<sub>2<\/sub>.\u00a0<em>Ab initio<\/em>\u00a0molecular dynamics simulations of the active species showed that free rotation of the Mn(CO)<sub>3<\/sub>\u00a0moiety allows for the approach of the protonated amine to the reactive center yielding a Mn-hydride intermediate, which is the key in the formation of H<sub>2<\/sub>\u00a0and HCOOH. Additional studies with DFT methods showed that the macrocyclic moiety hinders the insertion of CO<sub>2<\/sub>\u00a0to the metal hydride favoring the formation of H<sub>2<\/sub>\u00a0over HCOOH. Further, our results suggest that the minor CO product observed experimentally is formed when CO<sub>2<\/sub>\u00a0adds to Mn on the side opposite to the amine ligand before protonation. These results show how product selectivity can be modulated by ligand design in Mn-based catalysts, providing atomistic details that can be leveraged in the development of a fully selective system.<\/p>\n\n\n\n<p>Find a list of publications by\u00a0NordCO<sub>2<\/sub>\u00a0members on our\u00a0<a href=\"https:\/\/site.uit.no\/nordco2\/publications\/\">Publications<\/a>\u00a0page\u00a0\ud83d\ude42<\/p>\n","protected":false},"excerpt":{"rendered":"<p>Title:Exploring the Parameters Controlling Product Selectivity in Electrochemical CO2\u00a0Reduction in Competition with Hydrogen Evolution Employing Manganese Bipyridine Complexes Abstract:Selective reduction of CO2\u00a0is an efficient solution &hellip;<\/p>\n","protected":false},"author":514,"featured_media":0,"comment_status":"closed","ping_status":"closed","sticky":false,"template":"","format":"image","meta":{"ngg_post_thumbnail":0,"footnotes":""},"categories":[8],"tags":[],"class_list":["post-2948","post","type-post","status-publish","format-image","hentry","category-research","post_format-post-format-image"],"_links":{"self":[{"href":"https:\/\/site.uit.no\/nordco2\/wp-json\/wp\/v2\/posts\/2948","targetHints":{"allow":["GET"]}}],"collection":[{"href":"https:\/\/site.uit.no\/nordco2\/wp-json\/wp\/v2\/posts"}],"about":[{"href":"https:\/\/site.uit.no\/nordco2\/wp-json\/wp\/v2\/types\/post"}],"author":[{"embeddable":true,"href":"https:\/\/site.uit.no\/nordco2\/wp-json\/wp\/v2\/users\/514"}],"replies":[{"embeddable":true,"href":"https:\/\/site.uit.no\/nordco2\/wp-json\/wp\/v2\/comments?post=2948"}],"version-history":[{"count":1,"href":"https:\/\/site.uit.no\/nordco2\/wp-json\/wp\/v2\/posts\/2948\/revisions"}],"predecessor-version":[{"id":2950,"href":"https:\/\/site.uit.no\/nordco2\/wp-json\/wp\/v2\/posts\/2948\/revisions\/2950"}],"wp:attachment":[{"href":"https:\/\/site.uit.no\/nordco2\/wp-json\/wp\/v2\/media?parent=2948"}],"wp:term":[{"taxonomy":"category","embeddable":true,"href":"https:\/\/site.uit.no\/nordco2\/wp-json\/wp\/v2\/categories?post=2948"},{"taxonomy":"post_tag","embeddable":true,"href":"https:\/\/site.uit.no\/nordco2\/wp-json\/wp\/v2\/tags?post=2948"}],"curies":[{"name":"wp","href":"https:\/\/api.w.org\/{rel}","templated":true}]}}