Pan Lu, Gui-Min Kim, Nianfang Wang, Joongjai Panpranot, Whi Dong Kim, Doh C. Lee
{"title":"利用半胱胺钝化的铂沉积 CdS 纳米片选择性光催化 C-C 偶联苯甲醇制氢苯甲酸酯","authors":"Pan Lu, Gui-Min Kim, Nianfang Wang, Joongjai Panpranot, Whi Dong Kim, Doh C. Lee","doi":"10.1039/d4nr03148b","DOIUrl":null,"url":null,"abstract":"Achieving high selectivity towards hydrobenzoin (HB) from photocatalytic carbon-carbon (C-C) coupling reaction of benzyl alcohol (BzOH) remains a challenge due to side competing reactions and subsequent conversions of HB into its derivatives. In this study, we have developed a high-performance CdS-based photocatalyst for synthesizing HB with precisely controlled surface properties and structure, achieving high selectivity for HB synthesis. We employed strategies such as cysteamine passivation and Pt deposition to address issues related to photogenerated charge trapping and recombination, thereby enhancing the photocatalytic capability of CdS. With optimized Pt/CdS NSs as the photocatalyst, we investigated the impact of the Pt/CdS heterostructure on intermediate reactions, which in turn altered product selectivity. Specifically, excessive Pt suppresses the electron-induced benzaldehyde-to-intermediate reaction by consuming electrons for competing hydrogen evolution reaction (HER), leading to high selectivity toward benzaldehyde. In contrast, bare CdS without Pt suffers from insufficient charge supply for BzOH conversion due to the charge recombination issue, which promotes the subsequent conversion of HB to its derivatives. Notably, when Pt is precisely loaded to avoid dominant HER competition, the overall reaction rate increases, maintaining high selectivity towards HB and ensuring faster conversion of BzOH to HB rather than subsequent conversions of HB into its derivatives, thereby maximizing the HB yield. Subsequently, we have developed a photocatalyst that achieves a 93.4% conversion of 0.24 mmol BzOH with 85.3% selectivity toward HB under solar simulator irradiation (AM 1.5G). This work is expected to offer instructive guidance on rationally designing the photocatalyst for efficient C-C coupling reactions.","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":null,"pages":null},"PeriodicalIF":5.8000,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Selective photocatalytic C-C coupling of benzyl alcohol into hydrobenzoin using Pt-deposited CdS nanosheets passivated with cysteamine\",\"authors\":\"Pan Lu, Gui-Min Kim, Nianfang Wang, Joongjai Panpranot, Whi Dong Kim, Doh C. Lee\",\"doi\":\"10.1039/d4nr03148b\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Achieving high selectivity towards hydrobenzoin (HB) from photocatalytic carbon-carbon (C-C) coupling reaction of benzyl alcohol (BzOH) remains a challenge due to side competing reactions and subsequent conversions of HB into its derivatives. In this study, we have developed a high-performance CdS-based photocatalyst for synthesizing HB with precisely controlled surface properties and structure, achieving high selectivity for HB synthesis. We employed strategies such as cysteamine passivation and Pt deposition to address issues related to photogenerated charge trapping and recombination, thereby enhancing the photocatalytic capability of CdS. With optimized Pt/CdS NSs as the photocatalyst, we investigated the impact of the Pt/CdS heterostructure on intermediate reactions, which in turn altered product selectivity. Specifically, excessive Pt suppresses the electron-induced benzaldehyde-to-intermediate reaction by consuming electrons for competing hydrogen evolution reaction (HER), leading to high selectivity toward benzaldehyde. In contrast, bare CdS without Pt suffers from insufficient charge supply for BzOH conversion due to the charge recombination issue, which promotes the subsequent conversion of HB to its derivatives. Notably, when Pt is precisely loaded to avoid dominant HER competition, the overall reaction rate increases, maintaining high selectivity towards HB and ensuring faster conversion of BzOH to HB rather than subsequent conversions of HB into its derivatives, thereby maximizing the HB yield. Subsequently, we have developed a photocatalyst that achieves a 93.4% conversion of 0.24 mmol BzOH with 85.3% selectivity toward HB under solar simulator irradiation (AM 1.5G). 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Selective photocatalytic C-C coupling of benzyl alcohol into hydrobenzoin using Pt-deposited CdS nanosheets passivated with cysteamine
Achieving high selectivity towards hydrobenzoin (HB) from photocatalytic carbon-carbon (C-C) coupling reaction of benzyl alcohol (BzOH) remains a challenge due to side competing reactions and subsequent conversions of HB into its derivatives. In this study, we have developed a high-performance CdS-based photocatalyst for synthesizing HB with precisely controlled surface properties and structure, achieving high selectivity for HB synthesis. We employed strategies such as cysteamine passivation and Pt deposition to address issues related to photogenerated charge trapping and recombination, thereby enhancing the photocatalytic capability of CdS. With optimized Pt/CdS NSs as the photocatalyst, we investigated the impact of the Pt/CdS heterostructure on intermediate reactions, which in turn altered product selectivity. Specifically, excessive Pt suppresses the electron-induced benzaldehyde-to-intermediate reaction by consuming electrons for competing hydrogen evolution reaction (HER), leading to high selectivity toward benzaldehyde. In contrast, bare CdS without Pt suffers from insufficient charge supply for BzOH conversion due to the charge recombination issue, which promotes the subsequent conversion of HB to its derivatives. Notably, when Pt is precisely loaded to avoid dominant HER competition, the overall reaction rate increases, maintaining high selectivity towards HB and ensuring faster conversion of BzOH to HB rather than subsequent conversions of HB into its derivatives, thereby maximizing the HB yield. Subsequently, we have developed a photocatalyst that achieves a 93.4% conversion of 0.24 mmol BzOH with 85.3% selectivity toward HB under solar simulator irradiation (AM 1.5G). This work is expected to offer instructive guidance on rationally designing the photocatalyst for efficient C-C coupling reactions.
期刊介绍:
Nanoscale is a high-impact international journal, publishing high-quality research across nanoscience and nanotechnology. Nanoscale publishes a full mix of research articles on experimental and theoretical work, including reviews, communications, and full papers.Highly interdisciplinary, this journal appeals to scientists, researchers and professionals interested in nanoscience and nanotechnology, quantum materials and quantum technology, including the areas of physics, chemistry, biology, medicine, materials, energy/environment, information technology, detection science, healthcare and drug discovery, and electronics.