Interface Synergy of Exposed Oxygen Vacancy and Pd Lewis Acid Sites Enabling Superior Cooperative Photoredox Synthesis
Zhi-Sang Huang
College of Chemistry, State Key Laboratory of Photocatalysis on Energy and Environment, Fuzhou University, 350116 Fuzhou, China
Search for more papers by this authorYin-Feng Wang
College of Chemistry, State Key Laboratory of Photocatalysis on Energy and Environment, Fuzhou University, 350116 Fuzhou, China
Search for more papers by this authorDr. Ming-Yu Qi
Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, 611731 Chengdu, China
Search for more papers by this authorDr. Marco Conte
Department of Chemistry, University of Sheffield, S3 7HF Sheffield, UK
Search for more papers by this authorProf. Dr. Zi-Rong Tang
College of Chemistry, State Key Laboratory of Photocatalysis on Energy and Environment, Fuzhou University, 350116 Fuzhou, China
Search for more papers by this authorCorresponding Author
Prof. Dr. Yi-Jun Xu
College of Chemistry, State Key Laboratory of Photocatalysis on Energy and Environment, Fuzhou University, 350116 Fuzhou, China
Search for more papers by this authorZhi-Sang Huang
College of Chemistry, State Key Laboratory of Photocatalysis on Energy and Environment, Fuzhou University, 350116 Fuzhou, China
Search for more papers by this authorYin-Feng Wang
College of Chemistry, State Key Laboratory of Photocatalysis on Energy and Environment, Fuzhou University, 350116 Fuzhou, China
Search for more papers by this authorDr. Ming-Yu Qi
Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, 611731 Chengdu, China
Search for more papers by this authorDr. Marco Conte
Department of Chemistry, University of Sheffield, S3 7HF Sheffield, UK
Search for more papers by this authorProf. Dr. Zi-Rong Tang
College of Chemistry, State Key Laboratory of Photocatalysis on Energy and Environment, Fuzhou University, 350116 Fuzhou, China
Search for more papers by this authorCorresponding Author
Prof. Dr. Yi-Jun Xu
College of Chemistry, State Key Laboratory of Photocatalysis on Energy and Environment, Fuzhou University, 350116 Fuzhou, China
Search for more papers by this authorAbstract
Photo-driven cross-coupling of o-arylenediamines and alcohols has emerged as an alternative for the synthesis of bio-active benzimidazoles. However, tackling the key problem related to efficient adsorption and activation of both coupling partners over photocatalysts towards activity enhancement remains a challenge. Here, we demonstrate an efficient interface synergy strategy by coupling exposed oxygen vacancies (VO) and Pd Lewis acid sites for benzimidazole and hydrogen (H2) coproduction over Pd-loaded TiO2 nanospheres with the highest photoredox activity compared to previous works so far. The results show that the introduction of VO optimizes the energy band structure and supplies coordinatively unsaturated sites for adsorbing and activating ethanol molecules, affording acetaldehyde active intermediates. Pd acts as a Lewis acid site, enhancing the adsorption of alkaline amine molecules via Lewis acid-base pair interactions and driving the condensation process. Furthermore, VO and Pd synergistically promote interfacial charge transfer and separation. This work offers new insightful guidance for the rational design of semiconductor-based photocatalysts with interface synergy at the molecular level towards the high-performance coproduction of renewable fuels and value-added feedstocks.
Conflict of Interests
The authors declare no conflict of interest.
Open Research
Data Availability Statement
The data that support the findings of this study are available from the corresponding author upon reasonable request.
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