<br>碳空位引导双镍氮化碳光催化活性,Advanced Science

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碳空位引导双镍氮化碳光催化活性
Advanced Science ( IF 14.3 ) Pub Date : 2023-07-06 , DOI: 10.1002/advs.202303781
Miriam Marchi ₁ , Edoardo Raciti ₂ , Sai Manoj Gali ₂ , Federica Piccirilli ₃ , Hendrik Vondracek ₃ , Arianna Actis ₄ , Enrico Salvadori ₄ , Cristian Rosso ₁ , Alejandro Criado ₅ , Carmine D'Agostino _{6,

7} , Luke Forster ₆ , Daniel Lee ₆ , Alexandre C Foucher ₈ , Rajeev Kumar Rai ₈ , David Beljonne ₂ , Eric A Stach ₈ , Mario Chiesa ₄ , Roberto Lazzaroni ₂ , Giacomo Filippini ₁ , Maurizio Prato _{1,

9,

10} , Michele Melchionna ₁ , Paolo Fornasiero _{1,

11}

Affiliation

Department of Chemical and Pharmaceutical Sciences, Center for Energy, Environment and Transport "Giacomo Ciamician", INSTM UdR Trieste, University of Trieste, Via Licio Giorgieri 1, Trieste, 34127, Italy.
Laboratory for Chemistry of Novel Materials, Materials Research Institute, University of Mons-UMONS, Mons, 7000, Belgium.
Elettra Sincrotrone Trieste, Strada Statale 14 km 163.5 in Area Science Park Basovizza, Trieste, 34149, Italy.
Department of Chemistry and NIS Centre, University of Torino, Via Pietro Giuria 7, Torino, 10125, Italy.
Centro Interdisciplinar de Química e Bioloxía-CICA, Universidade da Coruña, Rúa As Carballeiras, A Coruña, 15071, Spain.
Department of Chemical Engineering, The University of Manchester, Oxford Road, Manchester, M13 9PL, UK.
Department of Civil, Chemical, Environmental and Material Engineering (DICAM), Alma Mater Studiorum, University of Bologna, Via Terracini, 28, Bologna, 40131, Italy.
Department of Materials Science and Engineering, University of Pennsylvania, Philadelphia, PA, 19104-6272, USA.
Center for Cooperative Research in Biomaterials (CIC biomaGUNE), Basque Research and Technology Alliance (BRTA), Paseo de Miramón 194, Donostia-San Sebastián, 20014, Spain.
Ikerbasque, Basque Foundation for Science, Bilbao, 48013, Spain.
ICCOM-CNR, Unit of Trieste, via L. Giorgieri 1, Trieste, 34127, Italy.

氮化碳（CN）结构的操控是增强CN基光催化剂活性的主要途径之一。提高光催化异质材料的效率是实现有机合成可持续方案的关键一步。然而，对与细微结构变化相关的结构/活性关系的了解有限，阻碍了新型光催化材料的完全合理设计，限制了实际应用。在这里，CN结构是通过微波处理来设计的，材料的结构围绕其适合Ni双光催化的功能进行塑造，从而提高了反应效率，朝向许多CX （X=N，S），O）联轴器。先进的表征技术和第一原理模拟的结合表明，这种增强的反应性是由于碳空位的形成，碳空位演变成三唑和亚胺N物种，能够适当地结合Ni配合物并利用高效的双重催化作用。这里提出的具有成本效益的微波处理似乎是一种通用且可持续的方法，用于设计用于各种工业相关有机合成反应的 CN 基光催化剂。

"点击查看英文标题和摘要"

Carbon Vacancies Steer the Activity in Dual Ni Carbon Nitride Photocatalysis

The manipulation of carbon nitride (CN) structures is one main avenue to enhance the activity of CN-based photocatalysts. Increasing the efficiency of photocatalytic heterogeneous materials is a critical step toward the realistic implementation of sustainable schemes for organic synthesis. However, limited knowledge of the structure/activity relationship in relation to subtle structural variations prevents a fully rational design of new photocatalytic materials, limiting practical applications. Here, the CN structure is engineered by means of a microwave treatment, and the structure of the material is shaped around its suitable functionality for Ni dual photocatalysis, with a resulting boosting of the reaction efficiency toward many CX (X = N, S, O) couplings. The combination of advanced characterization techniques and first-principle simulations reveals that this enhanced reactivity is due to the formation of carbon vacancies that evolve into triazole and imine N species able to suitably bind Ni complexes and harness highly efficient dual catalysis. The cost-effective microwave treatment proposed here appears as a versatile and sustainable approach to the design of CN-based photocatalysts for a wide range of industrially relevant organic synthetic reactions.

更新日期：2023-07-06

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