Deciphering Catalytic Selectivity on Uneven Terraces

نویسندگان

چکیده

Understanding the relationship between catalytic selectivity and surface structures of heterogeneous catalysts is essential for high-performance catalysis. In this issue Chem, Zhu et al. report a puzzle-solving strategy relying on single-crystal foils Pearson correlation analysis to determine dependence activity principal parameters. Heterogeneous catalysis solid surfaces represents most pervasive interdisciplinary science influencing chemical industry perhaps having significant societal impact, although its importance often underestimated or even hidden. For example, converting carbon dioxide (CO2) into carbon-containing chemicals fuels important in industrial sustainability environmental protection. Electrochemical CO2 reduction reaction (eCO2RR) aqueous electrolyte has shown great promise synthesizing various by using metal nanostructures as enhance kinetics product selectivity. Metal nanoparticles with well-controlled compositions,1Kim D. Xie C. Becknell N. Yu Y. Karamad M. Chan K. Crumlin E.J. Nørskov J.K. Yang P. activation through atomic ordering transformations AuCu nanoparticles.J. Am. Chem. Soc. 2017; 139: 8329-8336Crossref PubMed Scopus (328) Google Scholar sizes,2Zhu W. Michalsky R. Metin Ö. Lv H. Guo S. Wright C.J. Sun X. Peterson A.A. Monodisperse Au selective electrocatalytic CO.J. 2013; 135: 16833-16836Crossref (865) shapes,3Liu Tao Zeng L. Liu Q. Xu Z. Luo J.L. Shape-dependent CO triangular silver nanoplates.J. 2160-2163Crossref (338) crystalline defects4Hu F. Abeyweera S.C. J. Zhang Wang Yan Quantifying twin boundaries.Chem. 2020; 6: 3007-3021Abstract Full Text PDF (11) Scholar,5Mariano R.G. McKelvey White H.S. Kanan M.W. Selective increase electroreduction at grain-boundary terminations.Science. 358: 1187-1192Crossref (354) have been extensively evaluated catalyzing eCO2RR. The studies highlight how these volume-dependent parameters influence performance nanoparticles. However, catalyst crucial determining given that only catalyst’s can interact reactants intermediates desirable reactions. It becomes develop direct surface. inhomogeneity nanoparticles, which usually exhibit multiple types not-well-described atoms, makes it challenging extract reliable structure-performance relationship. co-workers synthesis large-area copper (Cu) well-defined be described (or descriptors) such low-index crystal terraces (i.e., (111), (100), (110) facets; Figure 1A), coordination number step-terrace angle.6Zhu Zhong Hsu C.-S. Li Zhao Chen al.Product-specific active site motifs Cu electrochemical reduction.Chem. 2021; 7: 406-420Abstract (15) According microfacet notation,7Van Hove M.A. Somorjai G.A. A new notation high-Miller-index cubic materials terrace, step kink structures.Surf. Sci. 1980; 92: 489-518Crossref (201) each decomposed combination facets different constitution ratios, defines aforementioned descriptors. instance, high-index Cu(553) (S)-[33(111) + 21(110)], indicating (553) unit cell contains three (111) one (Figure 1B). dominating cells minor represent microscopic steps, angle. inclusion microfacets results collection atoms numbers, i.e., 9 terrace 7 11 atoms. Surface any descriptors, terraces, number, All contact contribute overall activity, variation descriptors influences foil. Deconvoluting impact descriptor but guiding design appropriate structures. used analyze preference eCO2RR products (e.g., C1 CO, HCOO−, CH4; C2+ C2H4, C2H5OH, n-C3H7OH) cathodic potentials. map configurations presented 1C, highlighting topological foils. coefficient value −1 1) shows two variables, generation specific more positive indicates higher product, negative stronger tendency suppress product. At low voltage (−0.95 V versus reversible hydrogen electrode [RHE]), Cu(111), Cu(100), Cu(110) favor production respectively top left). Increasing −1.15 changes Cu(111) CH4 does not Cu(100) significantly right). coefficients indicate both are favorable producing C2H5OH. Therefore, good selectively ethanol should expose much eliminate terraces. similar reveals regardless middle). reported paper provides promising understanding relationships. This ready extend kind surface, reactions catalyzed. resulting relationships will provide knowledge help performance. also standard calibrating fidelity theoretical calculations predictions. Product-Specific Active Site Motifs ReductionZhu al.ChemNovember 11, 2020In BriefWe rationally designed fabricated nine orientations electrocatalysts operandoly monitored their reconstructions. Quantitative correlations selectivities toward were established. We extracted distinct structural including facet, angle, reveal intrinsic structure-function uniquely identify product-producing sites CO2R. Full-Text

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ژورنال

عنوان ژورنال: Chem

سال: 2021

ISSN: ['2451-9308', '2451-9294']

DOI: https://doi.org/10.1016/j.chempr.2021.01.004