Harnessing strong metal–support interactions via a reverse route

Wu, Peiwen; Tan, Shuai; Moon, Jisue; Yan, Zihao; Fung, Victor; Li, Na; Yang, Shize; Cheng, Yongqiang; Abney, Carter W.; Wu, Zili; Savara, Aditya; Momen, Ayyoub Mehdizadeh; Jiang, De‐en; Su, Dong; Li, Huaming; Zhu, Wenshuai; Dai, Sheng; Zhu, Huiyuan

doi:10.1038/s41467-020-16674-y

Cited by 115 publications

(103 citation statements)

References 57 publications

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“…Regarding the materials system, metals confined in other materials systems beyond CNTs will open new opportunities in precisely tailoring the interplay between active sites and their microenvironment. For example, CNTs usually demonstrate weak interactions with metal centers; while metal oxides may establish strong-metal support interactions at the interface between oxides and metals, 97,98 enabling efficient charge transfer. We also anticipate that by reducing the size of the microenvironment imposed by the cover, the confinement effect may be amplified.…”

Section: Challenges and Opportunitiesmentioning

confidence: 99%

Electrocatalysis in confined spaces: interplay between well-defined materials and the microenvironment

et al. 2021

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Section: Challenges and Opportunitiesmentioning

confidence: 99%

Electrocatalysis in confined spaces: interplay between well-defined materials and the microenvironment

et al. 2021

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“… 13 − 15 The polymeric semiconductor graphitic carbon nitride (C 3 N 4 ) is, in fact, an optimal scaffold due to its nitrogen-rich structure. The inherent nitrogen-lined pores can accommodate the metal single atoms in a stable manner 16 via “strong metal–support interaction” (SMSI), 17 , 18 and this can enhance the photocatalytic performance. Carbon nitrides and Ni salts have been elegantly employed in photoredox catalysis.…”

Section: Introductionmentioning

confidence: 99%

Ligand–Metal Charge Transfer Induced via Adjustment of Textural Properties Controls the Performance of Single-Atom Catalysts during Photocatalytic Degradation

Liu

Zou

Cruz

et al. 2021

ACS Appl. Mater. Interfaces

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Because of their peculiar nitrogen-rich structure, carbon nitrides are convenient polydentate ligands for designing single atom-dispersed photocatalysts. However, the relation between catalysts’ textural properties and their photophysical–photocatalytic properties is rarely elaborated. Herein, we report the preparation and characterization of a series of single-atom heterogeneous catalysts featuring highly dispersed Ag and Cu species on mesoporous graphitic C 3 N 4 . We show that adjustment of materials textural properties and therefore metal single-atom coordination mode enables ligand-to-metal charge transfer (LMCT) or ligand-to-metal-to-ligand charge transfer (LMLCT), properties that were long speculated in single-atom catalysis but never observed. We employ the developed materials in the degradation of organic pollutants under irradiation with visible light. Kinetic investigations under flow conditions show that single atoms of Ag and Cu decrease the number of toxic organic fragmentation products while leading to a higher selectivity toward full degradation. The results correlate with the selected mode of charge transfer in the designed photocatalysts and provide a new understanding of how the local environment of a single-atom catalyst affects the surface structure and reactivity. The concepts can be exploited further to rationally design and optimize other single-atom materials.

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“…The metal-support interface regulates the catalytic properties by several ways, for example modifying electronic and geometric parameters; the former characterized by charge transfer between the metal sites and the support, while the latter, by decoration or coverage of metal sites by the support [25]. The classical strong metal-support interaction (SMSI) identified by Tauser and co-workers [26], involved noble metals supported on a reducible substrate (the representative example is TiO2) [27,28]; the partial reduction of the support at high temperatures severely affected the chemisorptive properties of the metal.…”

Section: Introductionmentioning

confidence: 99%

Pt-based Catalysts in the Dry Reforming of Methane: Effect of Support and Metal Precursor on the Catalytic Stability

et al. 2021

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Abstract. Platinum catalysts (1.5 wt. %) supported over CeO2 and γ-Al2O3 were synthesized via wet impregnation using two different Pt precursors: H2PtCl6 and Pt(acac)2. Catalysts were tested in the dry reforming of methane (DRM) reaction at stoichiometric conditions (CH4/CO2 molar ratio of 1) with two approaches: as a function of temperature (400-800 °C) and as a function of time on-stream (800 °C / 24 h). Platinum supported over ceria catalysts showed better catalytic properties, especially in the stability tests, where deactivation was almost negligible. In contrast, alumina-supported catalysts stability was considerably lower due to the increased formation of carbon residues and the significant Pt particle sintering after reaction at 800 °C for 24 h. Through different characterization techniques (TEM, CO chemisorption), a strong Pt-Ceria interaction was evidenced, which helped in preventing Pt particle agglomeration under reaction conditions and promoted active interface sites. Both features are proposed to be responsible for the Pt/CeO2 catalysts better catalytic performance. The effect of the Pt precursor depends on the nature of the support. In ceria, Cl species benefited the generation of oxygen vacancies and surface ceria reducibility; both features are responsible for the Pt/CeO2 anti-coke properties, thus impacting positively in the catalytic performance of the Pt(-cl)/Ce sample. Conversely, in alumina, these Cl species triggered particle sintering and carbon deposition during the DRM reaction, affecting the Pt(-cl)/Al catalytic performance. Resumen. Catalizadores de platino (1.5 % en peso) soportados sobre CeO2 y γ-Al2O3 fueron sintetizados mediante impregnación húmeda utilizando dos diferentes precursores de Pt: H2PtCl6 and Pt(acac)2. Los catalizadores fueron evaluados en la reacción de reformado seco de metano (DRM) en condiciones estequiométricas (razón molar de CH4/CO2 igual a 1) y con dos metodologías: en función de la temperatura de reacción (400-800 °C) y en función del tiempo de reacción (800 °C / 24 h). Los catalizadores de platino soportados sobre ceria mostraron las mejores propiedades catalíticas, especialmente en las pruebas de estabilidad, donde la desactivación fue muy baja. Por el contrario, la estabilidad catalítica de las muestras soportadas en alúmina fue considerablemente menor, debido tanto a la formación de residuos de carbón como al sinterizado de partículas de Pt. Por medio diferentes técnicas de caracterización (TEM, Quimisorción de CO), se evidenció una fuerte interacción Pt-Ceria, la cual ayudó a prevenir la aglomeración de partículas de Pt durante la reacción, además de promover la generación de sitios activos interfaciales. Ambas características se proponen como las responsables de las mejores propiedades catalíticas presentadas por los catalizadores Pt/CeO2. El efecto del precursor del Pt depende de la naturaleza del soporte. En ceria, las especies de cloro beneficiaron la generación de sitios vacantes de oxígeno así como la reducción superficial de la ceria; ambas características son responsables de las propiedades anti-coque en el sistema Pt/CeO2, por lo tanto, estas impactaron positivamente en el desempeño catalítico de la muestra Pt(-cl)/Ce. Por el contrario, en la alúmina, estas especies cloradas aparentemente promovieron el sinterizado de partículas y los depósitos de carbono durante la reacción, lo cual afectó el desempeño catalítico de la muestra Pt(-cl)/Al.

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Harnessing strong metal–support interactions via a reverse route

Cited by 115 publications

References 57 publications

Electrocatalysis in confined spaces: interplay between well-defined materials and the microenvironment

Electrocatalysis in confined spaces: interplay between well-defined materials and the microenvironment

Ligand–Metal Charge Transfer Induced via Adjustment of Textural Properties Controls the Performance of Single-Atom Catalysts during Photocatalytic Degradation

Pt-based Catalysts in the Dry Reforming of Methane: Effect of Support and Metal Precursor on the Catalytic Stability

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