{"id":319,"date":"2021-12-20T11:27:57","date_gmt":"2021-12-20T10:27:57","guid":{"rendered":"https:\/\/perso.ens-lyon.fr\/carine.michel\/?page_id=319"},"modified":"2021-12-20T11:40:04","modified_gmt":"2021-12-20T10:40:04","slug":"understanding-the-impact-of-water-on-the-catalytic-activity-and-stability","status":"publish","type":"page","link":"https:\/\/perso.ens-lyon.fr\/carine.michel\/research\/understanding-the-impact-of-water-on-the-catalytic-activity-and-stability\/","title":{"rendered":"Understanding the impact of water on the catalytic activity and stability"},"content":{"rendered":"

Inspired by my past work in solvent effects in organic reactivity, I have transferred the micro-solvation approach used in homogeneous phase to surface reactions aiming at understanding the role of water on the C-H and O-H scissions in alcohols [1<\/a>]: H-bonded water strongly activates the O-H scission but does not affect the C-H scission on Rh. This discovery immediately questioned the role of water on the activity of other metals. I evidenced that the impact of water depends on the oxophilicity of the metal: the stronger the oxophilicity, the stronger the impact. My collaborator A. Ruppert confirmed this prediction experimentally on the levulinic acid conversion into gamma-valerolactone.[2<\/a>] This collaborative work is an important milestone that put in evidence the importance of understanding the effect of water on the catalytic activity.<\/p>\n

The pH also affects the catalytic activity: to proceed efficiently, alcohol oxidation by O2<\/sub> using Au catalysts needs adding a base, which generates unwanted waste. Combining PCM and microsolvation, I included for the first time in a computational study the chemisorption of anionic hydroxide at the catalyst\/water interface. Rationalizing the role of the added base, I identified potential sources of improvement to guide the Catalysis community: the basic pH polarizes the metal surface and a similar effect can be achieved through alloying, additives and support effect.[3<\/a>]<\/p>\n

Water is detrimental to the stability of gamma-Al2<\/sub>O3<\/sub>, a widely-used support in metal-supported catalysts. Using ab initio metadynamics combined with experiments, I proposed a mechanism of a reaction of a surface in contact with water, mapped out the weak spots of gamma-Al2<\/sub>O3 <\/sub>and proposed a rational for the protection offered by the adsorption of polyols.[4<\/a>] This is one of the first examples of using this advanced simulation method to explore reactions at the solid\/liquid interface.<\/p>\n

References<\/strong><\/p>\n

    \n
  1. \u201cC-H versus O-H Bond Dissociation for Alcohols on a Rh(111) Surface: A Strong Assistance from Hydrogen Bonded Neighbors\u201d
    \nC. Michel<\/em>, F.\u00a0Auneau, F. Delbecq, and P. Sautet,     ACS Catal. 2011<\/a>, 1, 1430.<\/li>\n
  2. \u201cRole of water on metal catalyst performance for ketone hydrogenation. A join experimental and theoretical study on levulinic acid conversion into gamma-valerolactone,\u201d C. Michel, J. Zaffran, A. M. Ruppert, J. Matras-Michalska, M. Jedrzejczyk, J. Grams, P. Sautet
    \n    Chem. Comm. 2014<\/strong><\/a>, 50, 12450<\/li>\n
  3. \u201cUnraveling the Role of Base and Catalyst Polarization in Alcohol Oxidation on Au and Pt in Water\u00a0\u00bb
    \nGu, P. Sautet, and C. Michel<\/em>,     ACS Catal. 2018<\/strong><\/a>, 8, 11716.<\/li>\n
  4. \u201cReactivity of shape-controlled crystals and metadynamics simulations locate the weak spots of alumina in water\u00a0\u00bb
    \nR\u00e9ocreux, E. Girel, P. Clabaut, A. Tuel, M. Besson, A. Chaumonnot, A. Cabiac, P. Sautet, C. Michel<\/em>,     Nat. Comm. 2019<\/strong><\/a>, 10, 3139<\/li>\n<\/ol>\n","protected":false},"excerpt":{"rendered":"

    Inspired by my past work in solvent effects in organic reactivity, I have transferred the micro-solvation approach used in homogeneous phase to surface reactions aiming at understanding the role of water on the C-H and O-H scissions in alcohols [1]: H-bonded water strongly activates the O-H scission but does not affect the C-H scission on […]<\/p>\n","protected":false},"author":2,"featured_media":0,"parent":155,"menu_order":0,"comment_status":"closed","ping_status":"closed","template":"","meta":{"footnotes":""},"class_list":["post-319","page","type-page","status-publish","hentry"],"_links":{"self":[{"href":"https:\/\/perso.ens-lyon.fr\/carine.michel\/wp-json\/wp\/v2\/pages\/319","targetHints":{"allow":["GET"]}}],"collection":[{"href":"https:\/\/perso.ens-lyon.fr\/carine.michel\/wp-json\/wp\/v2\/pages"}],"about":[{"href":"https:\/\/perso.ens-lyon.fr\/carine.michel\/wp-json\/wp\/v2\/types\/page"}],"author":[{"embeddable":true,"href":"https:\/\/perso.ens-lyon.fr\/carine.michel\/wp-json\/wp\/v2\/users\/2"}],"replies":[{"embeddable":true,"href":"https:\/\/perso.ens-lyon.fr\/carine.michel\/wp-json\/wp\/v2\/comments?post=319"}],"version-history":[{"count":3,"href":"https:\/\/perso.ens-lyon.fr\/carine.michel\/wp-json\/wp\/v2\/pages\/319\/revisions"}],"predecessor-version":[{"id":323,"href":"https:\/\/perso.ens-lyon.fr\/carine.michel\/wp-json\/wp\/v2\/pages\/319\/revisions\/323"}],"up":[{"embeddable":true,"href":"https:\/\/perso.ens-lyon.fr\/carine.michel\/wp-json\/wp\/v2\/pages\/155"}],"wp:attachment":[{"href":"https:\/\/perso.ens-lyon.fr\/carine.michel\/wp-json\/wp\/v2\/media?parent=319"}],"curies":[{"name":"wp","href":"https:\/\/api.w.org\/{rel}","templated":true}]}}