Hui Bian , Xinyi Yuan , Nan Zhang , Zhuo Xu , Juhong Lian , Ruibin Jiang , Junqing Yan , Deng Li , Shengzhong (Frank) Liu
{"title":"Correlating vacancy-defect density with CO2 activation for promoted CO2 methanation over CsPbBr3 photocatalyst","authors":"Hui Bian , Xinyi Yuan , Nan Zhang , Zhuo Xu , Juhong Lian , Ruibin Jiang , Junqing Yan , Deng Li , Shengzhong (Frank) Liu","doi":"10.1016/j.cclet.2025.111034","DOIUrl":"10.1016/j.cclet.2025.111034","url":null,"abstract":"<div><div>Constructing vacancy-decorated metal halide perovskites (MHPs) have emerged as promising pathway to enhance photocatalytic activity and selectivity for solar CO<sub>2</sub> reduction. However, the controllable construction of vacancy defects is still challenging, and our understanding of the roles of these defects, particularly their effects on the adsorption activation of surface reaction molecules, is still insufficient. Herein, we elaborately designed and synthesized adjustable Br vacancies in CsPbBr<sub>3</sub> catalysts by manipulating the dissolution and recrystallization speed of precursors during the ball milling process using solvents with gradient polarities. We found that the Br vacancies could promote the charge separation, while having slight influence on the band structure of CsPbBr<sub>3</sub>. More importantly, temperature-programmed desorption results combined with theoretical calculations revealed that Br vacancies can significantly enhance the adsorption of CO<sub>2</sub> and CO on the surface, specifically increasing the adsorption strength between CO and the active sites. This finding provides a substantial opportunity for achieving high activity and selectivity in photocatalytic CO<sub>2</sub> methanation. Accordingly, a high rate of CO<sub>2</sub> photoreduction to CH<sub>4</sub> up to 17.94 ± 0.81 μmol g<sup>-1</sup> h<sup>-1</sup> along with superior selectivity of 95.8% were acquired for CsPbBr<sub>3<img></sub>HX featuring with the richest Br vacancy defects, which is 18.9-fold compared that of CsPbBr<sub>3<img></sub>CAN with the lowest Br vacancy defects. This investigation deepens insights into action mechanism of defects on halide perovskites catalysts, offering a novel strategy for the high-effective conversion of CO<sub>2</sub> into valuable products.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 7","pages":"Article 111034"},"PeriodicalIF":9.4,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143928655","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Runzi Cao , Heng Shao , Xinjie Wang , Jian Wang , Enxiang Shang , Yang Li
{"title":"Photocatalytic production of high-value-added fuels from biodegradable PBAT by Nb2O5/GCN heterojunction catalyst: Performance and mechanism","authors":"Runzi Cao , Heng Shao , Xinjie Wang , Jian Wang , Enxiang Shang , Yang Li","doi":"10.1016/j.cclet.2025.111029","DOIUrl":"10.1016/j.cclet.2025.111029","url":null,"abstract":"<div><div>Photocatalysis holds great promise for the conversion of plastic waste into valuable chemicals. However, the conversion efficiency is constrained by the poor carriers' separation efficiency over the single component photocatalyst. Herein, we synthesized a novel type Ⅱ Nb<sub>2</sub>O<sub>5</sub>/GCN heterojunction to investigate its efficiency in the photocatalytic upcycling of polybutylene adipate/terephthalate (PBAT) microplastics (MPs) into acids and alcohols under visible light irradiation (100 mW/cm2). The findings indicate that the charge transfer within the type Ⅱ Nb<sub>2</sub>O<sub>5</sub>/GCN occurs from the conduction band of GCN to the conduction band of Nb<sub>2</sub>O<sub>5</sub>, thereby enhancing the separation efficiency of carriers Notably, the rates of ethanol and acetic acid generation from 1.5 mg/mL PBAT MPs treated with the 60 %Nb<sub>2</sub>O<sub>5</sub>/GCN photocatalyst were 21.8-fold and 1.8-fold higher, respectively, compared to those by Nb<sub>2</sub>O<sub>5</sub> alone. Density functional theory calculations demonstrate that the hydroxyl radicals (<sup>•</sup>OH) produced by the Nb<sub>2</sub>O<sub>5</sub>/GCN heterojunction cleaves the ester bond (O<img>C=O) of PBAT MP into the monomer. These monomers are subsequently converted into acids and alcohols through various reactions, including C<img>C bond cleavage, hydrodeoxygenation, and C<img>C bond coupling. This study highlights the effectiveness of heterojunction photocatalyst in converting PBAT MPs into valuable chemicals, thus significantly promoting advancements in bioplastics recycling.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 7","pages":"Article 111029"},"PeriodicalIF":9.4,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144105815","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Tianwen Chen , Chunqiang Cai , Li Chen , Yanlin Chen , Lichun Dong , Luxi Tan , Zitong Liu
{"title":"Novel vinylene-bridged covalent organic framework based on diketopyrrolopyrrole with exceptional photothermal properties","authors":"Tianwen Chen , Chunqiang Cai , Li Chen , Yanlin Chen , Lichun Dong , Luxi Tan , Zitong Liu","doi":"10.1016/j.cclet.2025.111028","DOIUrl":"10.1016/j.cclet.2025.111028","url":null,"abstract":"<div><div>Vinylene-bridged covalent organic frameworks (V-COFs), as fully conjugated polymer structures, offer promising prospects in optoelectronics. However, challenges such as poor bond reversibility and limited monomer availability persist. In this study, we introduce Ph-DPP-COF, synthesized from a diketopyrrolopyrrole (DPP) core with methyl groups <em>via</em> a Knoevenagel condensation reaction. The resulting material features an AA stacking mode, large nanopores, and broad light absorption across the ultraviolet to near-infrared spectrum. Notably, Ph-DPP-COF achieves a photothermal conversion efficiency of 53 % under 660 nm laser irradiation. Its exceptional mechanical processability also offers considerable plasticity for practical applications. These findings suggest that Ph-DPP-COF not only provides a novel approach for developing photothermal conversion materials but also holds promise for future energy conversion and storage technologies.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 7","pages":"Article 111028"},"PeriodicalIF":9.4,"publicationDate":"2025-03-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143934737","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Exploring the potential and challenges of molecular-squeeze adsorption in sponge-like crystals","authors":"Yujuan Zhou, Jie Yang","doi":"10.1016/j.cclet.2025.111004","DOIUrl":"10.1016/j.cclet.2025.111004","url":null,"abstract":"","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 6","pages":"Article 111004"},"PeriodicalIF":9.4,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143704877","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Reduction of methane emission from microbial fuel cells during sulfamethoxazole wastewater treatment","authors":"Shilong Li , Liang Duan , Qiusheng Gao , Hengliang Zhang","doi":"10.1016/j.cclet.2025.110997","DOIUrl":"10.1016/j.cclet.2025.110997","url":null,"abstract":"<div><div>Carbon emissions from wastewater treatment contribute to global warming and have received widespread attention. It is necessary to seek low-carbon wastewater treatment technologies. Microbial fuel cells (MFC) and osmotic microbial fuel cells (OsMFC) are low-carbon technologies that enable both wastewater treatment and energy recovery. In this study, MFC and OsMFC were used to treat sulfamethoxazole (SMX) wastewater, and direct carbon emissions during operation was <em>calculated. The highest SMX removal rate can reach about 40%. Simultaneously, the CH<sub>4</sub> emission factor was significantly reduced to less than 6 g CO<sub>2</sub>/kg of chemical oxygen demand. The accumulation of SMX-degrading bacteria competed with methanogens for carbon source utilization, leading to a significant decrease in the relative abundance of methanogens. It is hoped that this study can provide a sustainable approach to antibiotic wastewater treatment and promote the development of low-carbon wastewater treatment technologies.</em></div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 6","pages":"Article 110997"},"PeriodicalIF":9.4,"publicationDate":"2025-02-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143830256","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Palladium-catalyzed modular biomimetic synthesis of lignans derivatives","authors":"Junlong Tang, Yuhan Zhao, Yangbin Jin, Liren Zhang, Yuanfang Wang, Wanqing Wu, Huanfeng Jiang","doi":"10.1016/j.cclet.2025.110969","DOIUrl":"10.1016/j.cclet.2025.110969","url":null,"abstract":"<div><div>Lignans have been established as a privileged scaffold in drug discovery, particularly in anticancer and antioxidant properties. Concise and efficient construction of lignans and their derivatives in a single operation holds great medicinal significance for structure-activity relationship studies yet remains challenging. Drawing inspiration from the biosynthesis of lignans, we present a general, high-step-economy palladium-catalyzed reaction that converts simple chemical feedstocks into dehydrodibenzylbutyrolactone lignans through the <em>in-situ</em> construction and coupling of two phenylpropanoid molecules. The diversity of organoboronic acids and the editability of enyne provide a powerful platform for the rapid construction of lignan libraries, featuring 82 lignans analogs, collective syntheses of 10 distinct lignan skeletons, and 13 hybrid molecules combining pharmacophore fragments with drug and derivatives. The subtle combination of phosphine ligands with quinones for switching chemoselectivity is vital to the success of this protocol.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 7","pages":"Article 110969"},"PeriodicalIF":9.4,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143895991","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Phase diagram as a lens for unveiling thermodynamics trends in lithium–sulfur batteries","authors":"Bo-Bo Zou, Hong-Jie Peng","doi":"10.1016/j.cclet.2025.110986","DOIUrl":"10.1016/j.cclet.2025.110986","url":null,"abstract":"","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 7","pages":"Article 110986"},"PeriodicalIF":9.4,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144105816","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}