{"title":"Ionic Diffusion inCO2Adsorption byLi4SiO4: Inert-Marker Experiment and DFT Calculations","authors":"Tao Deng, Shuzhen Chen, Zongze Lv, Yujie Zheng, Shaojun Xu, Changlei Qin","doi":"10.1103/physrevlett.133.198001","DOIUrl":null,"url":null,"abstract":"<mjx-container ctxtmenu_counter=\"25\" ctxtmenu_oldtabindex=\"1\" jax=\"CHTML\" overflow=\"linebreak\" role=\"tree\" sre-explorer- style=\"font-size: 100.7%;\" tabindex=\"0\"><mjx-math data-semantic-structure=\"(2 0 1)\"><mjx-mrow><mjx-msub data-semantic-children=\"0,1\" data-semantic- data-semantic-owns=\"0 1\" data-semantic-role=\"unknown\" data-semantic-speech=\"upper C upper O 2\" data-semantic-type=\"subscript\"><mjx-mrow><mjx-mi data-semantic-font=\"normal\" data-semantic- data-semantic-parent=\"2\" data-semantic-role=\"unknown\" data-semantic-type=\"identifier\"><mjx-c noic=\"true\" style=\"padding-top: 0.669em;\">C</mjx-c><mjx-c style=\"padding-top: 0.669em;\">O</mjx-c></mjx-mi></mjx-mrow><mjx-script style=\"vertical-align: -0.15em;\"><mjx-mn data-semantic-annotation=\"clearspeak:simple\" data-semantic-font=\"normal\" data-semantic- data-semantic-parent=\"2\" data-semantic-role=\"integer\" data-semantic-type=\"number\" size=\"s\"><mjx-c>2</mjx-c></mjx-mn></mjx-script></mjx-msub></mjx-mrow></mjx-math></mjx-container> adsorption by <mjx-container ctxtmenu_counter=\"26\" ctxtmenu_oldtabindex=\"1\" jax=\"CHTML\" overflow=\"linebreak\" role=\"tree\" sre-explorer- style=\"font-size: 100.7%;\" tabindex=\"0\"><mjx-math data-semantic-structure=\"(7 (2 0 1) 6 (5 3 4))\"><mjx-mrow data-semantic-annotation=\"clearspeak:unit\" data-semantic-children=\"2,5\" data-semantic-content=\"6\" data-semantic- data-semantic-owns=\"2 6 5\" data-semantic-role=\"implicit\" data-semantic-speech=\"upper L i 4 upper S i upper O 4\" data-semantic-type=\"infixop\"><mjx-msub data-semantic-children=\"0,1\" data-semantic- data-semantic-owns=\"0 1\" data-semantic-parent=\"7\" data-semantic-role=\"unknown\" data-semantic-type=\"subscript\"><mjx-mrow><mjx-mi data-semantic-font=\"normal\" data-semantic- data-semantic-parent=\"2\" data-semantic-role=\"unknown\" data-semantic-type=\"identifier\"><mjx-c noic=\"true\" style=\"padding-top: 0.673em;\">L</mjx-c><mjx-c style=\"padding-top: 0.673em;\">i</mjx-c></mjx-mi></mjx-mrow><mjx-script style=\"vertical-align: -0.15em;\"><mjx-mn data-semantic-annotation=\"clearspeak:simple\" data-semantic-font=\"normal\" data-semantic- data-semantic-parent=\"2\" data-semantic-role=\"integer\" data-semantic-type=\"number\" size=\"s\"><mjx-c>4</mjx-c></mjx-mn></mjx-script></mjx-msub><mjx-mo data-semantic-added=\"true\" data-semantic- data-semantic-operator=\"infixop,\" data-semantic-parent=\"7\" data-semantic-role=\"multiplication\" data-semantic-type=\"operator\"><mjx-c></mjx-c></mjx-mo><mjx-msub data-semantic-children=\"3,4\" data-semantic- data-semantic-owns=\"3 4\" data-semantic-parent=\"7\" data-semantic-role=\"unknown\" data-semantic-type=\"subscript\"><mjx-mrow><mjx-mi data-semantic-font=\"normal\" data-semantic- data-semantic-parent=\"5\" data-semantic-role=\"unknown\" data-semantic-type=\"identifier\"><mjx-c noic=\"true\" style=\"padding-top: 0.673em;\">S</mjx-c><mjx-c noic=\"true\" style=\"padding-top: 0.673em;\">i</mjx-c><mjx-c style=\"padding-top: 0.673em;\">O</mjx-c></mjx-mi></mjx-mrow><mjx-script style=\"vertical-align: -0.15em;\"><mjx-mn data-semantic-annotation=\"clearspeak:simple\" data-semantic-font=\"normal\" data-semantic- data-semantic-parent=\"5\" data-semantic-role=\"integer\" data-semantic-type=\"number\" size=\"s\"><mjx-c>4</mjx-c></mjx-mn></mjx-script></mjx-msub></mjx-mrow></mjx-math></mjx-container> has garnered significant attention for its potential in effectively capturing <mjx-container ctxtmenu_counter=\"27\" ctxtmenu_oldtabindex=\"1\" jax=\"CHTML\" overflow=\"linebreak\" role=\"tree\" sre-explorer- style=\"font-size: 100.7%;\" tabindex=\"0\"><mjx-math data-semantic-structure=\"(2 0 1)\"><mjx-mrow><mjx-msub data-semantic-children=\"0,1\" data-semantic- data-semantic-owns=\"0 1\" data-semantic-role=\"unknown\" data-semantic-speech=\"upper C upper O 2\" data-semantic-type=\"subscript\"><mjx-mrow><mjx-mi data-semantic-font=\"normal\" data-semantic- data-semantic-parent=\"2\" data-semantic-role=\"unknown\" data-semantic-type=\"identifier\"><mjx-c noic=\"true\" style=\"padding-top: 0.669em;\">C</mjx-c><mjx-c style=\"padding-top: 0.669em;\">O</mjx-c></mjx-mi></mjx-mrow><mjx-script style=\"vertical-align: -0.15em;\"><mjx-mn data-semantic-annotation=\"clearspeak:simple\" data-semantic-font=\"normal\" data-semantic- data-semantic-parent=\"2\" data-semantic-role=\"integer\" data-semantic-type=\"number\" size=\"s\"><mjx-c>2</mjx-c></mjx-mn></mjx-script></mjx-msub></mjx-mrow></mjx-math></mjx-container>. The slow diffusion-controlled reaction within the product layer is a key factor affecting <mjx-container ctxtmenu_counter=\"28\" ctxtmenu_oldtabindex=\"1\" jax=\"CHTML\" overflow=\"linebreak\" role=\"tree\" sre-explorer- style=\"font-size: 100.7%;\" tabindex=\"0\"><mjx-math data-semantic-structure=\"(2 0 1)\"><mjx-mrow><mjx-msub data-semantic-children=\"0,1\" data-semantic- data-semantic-owns=\"0 1\" data-semantic-role=\"unknown\" data-semantic-speech=\"upper C upper O 2\" data-semantic-type=\"subscript\"><mjx-mrow><mjx-mi data-semantic-font=\"normal\" data-semantic- data-semantic-parent=\"2\" data-semantic-role=\"unknown\" data-semantic-type=\"identifier\"><mjx-c noic=\"true\" style=\"padding-top: 0.669em;\">C</mjx-c><mjx-c style=\"padding-top: 0.669em;\">O</mjx-c></mjx-mi></mjx-mrow><mjx-script style=\"vertical-align: -0.15em;\"><mjx-mn data-semantic-annotation=\"clearspeak:simple\" data-semantic-font=\"normal\" data-semantic- data-semantic-parent=\"2\" data-semantic-role=\"integer\" data-semantic-type=\"number\" size=\"s\"><mjx-c>2</mjx-c></mjx-mn></mjx-script></mjx-msub></mjx-mrow></mjx-math></mjx-container> adsorption. However, no research has been conducted to study the diffusion mechanism. Here, ionic diffusion was systematically comprehended through inert-marker experiments and first-principles calculations. An electron probe test clearly captures the movement of inert-marker Pt into the product layer, thus the outward transfer of <mjx-container ctxtmenu_counter=\"29\" ctxtmenu_oldtabindex=\"1\" jax=\"CHTML\" overflow=\"linebreak\" role=\"tree\" sre-explorer- style=\"font-size: 100.7%;\" tabindex=\"0\"><mjx-math data-semantic-structure=\"(4 0 (3 1 2))\"><mjx-mrow><mjx-msup data-semantic-children=\"0,3\" data-semantic- data-semantic-owns=\"0 3\" data-semantic-role=\"latinletter\" data-semantic-speech=\"normal upper O Superscript 2 minus\" data-semantic-type=\"superscript\"><mjx-mrow><mjx-mi data-semantic-annotation=\"clearspeak:simple\" data-semantic-font=\"normal\" data-semantic- data-semantic-parent=\"4\" data-semantic-role=\"latinletter\" data-semantic-type=\"identifier\"><mjx-c>O</mjx-c></mjx-mi></mjx-mrow><mjx-script style=\"vertical-align: 0.363em;\"><mjx-mrow data-semantic-children=\"1\" data-semantic-content=\"2\" data-semantic- data-semantic-owns=\"1 2\" data-semantic-parent=\"4\" data-semantic-role=\"subtraction\" data-semantic-type=\"postfixop\" size=\"s\"><mjx-mn data-semantic-annotation=\"clearspeak:simple\" data-semantic-font=\"normal\" data-semantic- data-semantic-parent=\"3\" data-semantic-role=\"integer\" data-semantic-type=\"number\"><mjx-c>2</mjx-c></mjx-mn><mjx-mo data-semantic- data-semantic-operator=\"postfixop,−\" data-semantic-parent=\"3\" data-semantic-role=\"subtraction\" data-semantic-type=\"operator\"><mjx-c>−</mjx-c></mjx-mo></mjx-mrow></mjx-script></mjx-msup></mjx-mrow></mjx-math></mjx-container> and <mjx-container ctxtmenu_counter=\"30\" ctxtmenu_oldtabindex=\"1\" jax=\"CHTML\" overflow=\"linebreak\" role=\"tree\" sre-explorer- style=\"font-size: 100.7%;\" tabindex=\"0\"><mjx-math data-semantic-structure=\"(2 0 1)\"><mjx-mrow><mjx-msup data-semantic-children=\"0,1\" data-semantic- data-semantic-owns=\"0 1\" data-semantic-role=\"unknown\" data-semantic-speech=\"upper L i Superscript plus\" data-semantic-type=\"superscript\"><mjx-mi data-semantic-font=\"normal\" data-semantic- data-semantic-parent=\"2\" data-semantic-role=\"unknown\" data-semantic-type=\"identifier\"><mjx-c noic=\"true\" style=\"padding-top: 0.673em;\">L</mjx-c><mjx-c style=\"padding-top: 0.673em;\">i</mjx-c></mjx-mi><mjx-script style=\"vertical-align: 0.4em;\"><mjx-mo data-semantic- data-semantic-parent=\"2\" data-semantic-role=\"addition\" data-semantic-type=\"operator\" size=\"s\"><mjx-c>+</mjx-c></mjx-mo></mjx-script></mjx-msup></mjx-mrow></mjx-math></mjx-container> ions is proposed to be the dominant diffusion mode. Density functional theory calculations also confirm the diffusion of <mjx-container ctxtmenu_counter=\"31\" ctxtmenu_oldtabindex=\"1\" jax=\"CHTML\" overflow=\"linebreak\" role=\"tree\" sre-explorer- style=\"font-size: 100.7%;\" tabindex=\"0\"><mjx-math data-semantic-structure=\"(4 0 (3 1 2))\"><mjx-mrow><mjx-msup data-semantic-children=\"0,3\" data-semantic- data-semantic-owns=\"0 3\" data-semantic-role=\"latinletter\" data-semantic-speech=\"normal upper O Superscript 2 minus\" data-semantic-type=\"superscript\"><mjx-mi data-semantic-annotation=\"clearspeak:simple\" data-semantic-font=\"normal\" data-semantic- data-semantic-parent=\"4\" data-semantic-role=\"latinletter\" data-semantic-type=\"identifier\"><mjx-c>O</mjx-c></mjx-mi><mjx-script style=\"vertical-align: 0.363em;\"><mjx-mrow data-semantic-children=\"1\" data-semantic-content=\"2\" data-semantic- data-semantic-owns=\"1 2\" data-semantic-parent=\"4\" data-semantic-role=\"subtraction\" data-semantic-type=\"postfixop\" size=\"s\"><mjx-mn data-semantic-annotation=\"clearspeak:simple\" data-semantic-font=\"normal\" data-semantic- data-semantic-parent=\"3\" data-semantic-role=\"integer\" data-semantic-type=\"number\"><mjx-c>2</mjx-c></mjx-mn><mjx-mo data-semantic- data-semantic-operator=\"postfixop,−\" data-semantic-parent=\"3\" data-semantic-role=\"subtraction\" data-semantic-type=\"operator\"><mjx-c>−</mjx-c></mjx-mo></mjx-mrow></mjx-script></mjx-msup></mjx-mrow></mjx-math></mjx-container> and <mjx-container ctxtmenu_counter=\"32\" ctxtmenu_oldtabindex=\"1\" jax=\"CHTML\" overflow=\"linebreak\" role=\"tree\" sre-explorer- style=\"font-size: 100.7%;\" tabindex=\"0\"><mjx-math data-semantic-structure=\"(2 0 1)\"><mjx-mrow><mjx-msup data-semantic-children=\"0,1\" data-semantic- data-semantic-owns=\"0 1\" data-semantic-role=\"unknown\" data-semantic-speech=\"upper L i Superscript plus\" data-semantic-type=\"superscript\"><mjx-mi data-semantic-font=\"normal\" data-semantic- data-semantic-parent=\"2\" data-semantic-role=\"unknown\" data-semantic-type=\"identifier\"><mjx-c noic=\"true\" style=\"padding-top: 0.673em;\">L</mjx-c><mjx-c style=\"padding-top: 0.673em;\">i</mjx-c></mjx-mi><mjx-script style=\"vertical-align: 0.4em;\"><mjx-mo data-semantic- data-semantic-parent=\"2\" data-semantic-role=\"addition\" data-semantic-type=\"operator\" size=\"s\"><mjx-c>+</mjx-c></mjx-mo></mjx-script></mjx-msup></mjx-mrow></mjx-math></mjx-container> with the former being the speed controlling step.","PeriodicalId":20069,"journal":{"name":"Physical review letters","volume":null,"pages":null},"PeriodicalIF":8.1000,"publicationDate":"2024-11-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Physical review letters","FirstCategoryId":"101","ListUrlMain":"https://doi.org/10.1103/physrevlett.133.198001","RegionNum":1,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"PHYSICS, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
Abstract
CO2 adsorption by Li4SiO4 has garnered significant attention for its potential in effectively capturing CO2. The slow diffusion-controlled reaction within the product layer is a key factor affecting CO2 adsorption. However, no research has been conducted to study the diffusion mechanism. Here, ionic diffusion was systematically comprehended through inert-marker experiments and first-principles calculations. An electron probe test clearly captures the movement of inert-marker Pt into the product layer, thus the outward transfer of O2− and Li+ ions is proposed to be the dominant diffusion mode. Density functional theory calculations also confirm the diffusion of O2− and Li+ with the former being the speed controlling step.
期刊介绍：
Physical review letters(PRL)covers the full range of applied, fundamental, and interdisciplinary physics research topics:
General physics, including statistical and quantum mechanics and quantum information
Gravitation, astrophysics, and cosmology
Elementary particles and fields
Nuclear physics
Atomic, molecular, and optical physics
Nonlinear dynamics, fluid dynamics, and classical optics
Plasma and beam physics
Condensed matter and materials physics
Polymers, soft matter, biological, climate and interdisciplinary physics, including networks
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