{"title":"Construction of piezoelectric photocatalyst Au/BiVO4 for efficient degradation of tetracycline and studied at single-particle level","authors":"Yujia Zhang, Yan Liu, Xueqin Gong, Zeyan Wang, Yuanyuan Liu, Peng Wang, Hefeng Cheng, Baibiao Huang, Zhaoke Zheng","doi":"10.20517/cs.2023.65","DOIUrl":"https://doi.org/10.20517/cs.2023.65","url":null,"abstract":"Piezopotential-assisted catalysis has been proven to be a low-cost and high-efficiency environmental purification process. Herein, Au/bismuth vanadate (BiVO4) piezoelectric photocatalysts are prepared by modifying highly dispersed Au nanoparticles (AuNPs) on piezoelectric BiVO4 microcrystal by a deposition-precipitation approach. Under visible light irradiation and assisted ultrasound excitation, the removal rate of tetracycline was 95% within 60 min, demonstrating the optimum photocatalytic performance over 3Au/BiVO4. The significantly enhanced photocatalytic performance is due to the synergistic coupling of plasmonic and piezotronic effect based on facet engineering. Single-particle spectroscopy technology can provide photoluminescence (PL) lifetime and PL spectra information in the micro-/nano regions, thereby exploring the charge transfer behavior of heterostructures. Single-particle PL images revealed a significant attenuation of PL emission and shortened PL lifetime of 3Au/BiVO4, compared with BiVO4, indicating that high-density dispersed AuNPs promote charge transfer. In situ monitoring of individual BiVO4 and 3Au/BiVO4 particles before and after polarization treatment confirms that the piezoelectric field of the BiVO4 decahedron further promotes separation of photogenerated carriers induced by plasmonic effect. Driven by the piezoelectric potential induced by ultrasonic vibration near the heterostructures, high-energy hot electrons excited on plasmonic AuNPs can be effectively extracted to BiVO4. This work provides new choices for designing high-performance pollutant treatment catalysts.","PeriodicalId":381136,"journal":{"name":"Chemical Synthesis","volume":"996 ","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140748965","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Xianchen Gong, Jie Tuo, Jilong Wang, Xintong Li, Chengwei Zhai, Hao Xu, Peng Wu
{"title":"Hydrophilic Ti-MWW for catalyzing epoxidation of allyl alcohol","authors":"Xianchen Gong, Jie Tuo, Jilong Wang, Xintong Li, Chengwei Zhai, Hao Xu, Peng Wu","doi":"10.20517/cs.2023.59","DOIUrl":"https://doi.org/10.20517/cs.2023.59","url":null,"abstract":"Titanosilicates are widely applied in the alkene epoxidation reactions with high reaction rate and selectivity to desired products. Their catalytic performance depends on the structure topology, the micro-environment of Ti active sites, and the hydrophobicity/hydrophilicity of zeolite framework. Herein, we focus on a hydrophilic substrate of allyl alcohol (AAL) and investigated catalytic performance of four titanosilicates (TS-1, Ti-MOR, Ti-MWW, and Re-Ti-MWW) in the AAL epoxidation reaction with hydrogen peroxide as the oxidant. Among them, Re-Ti-MWW, synthesized via the post-modification of Ti-MWW with piperidine, exhibited the highest activity. Moreover, the preferred solvent changed from MeCN for Ti-MWW to H2O for Re-Ti-MWW. The relative diffusion rate of AAL over Re-Ti-MWW was up to 466 × 10-7 s-1, much larger than those of other zeolites. The higher diffusion rate of Re-Ti-MWW was probably derived from the higher framework hydrophilicity as revealed by the smaller water contact angle of Re-Ti-MWW compared to the other zeolites, which contributed to the high activity in AAL epoxidation. In the continuous slurry reactor, Re-Ti-MWW achieved a high catalytic lifetime of 163 h, with the selectivity of desirable glycidol product maintained at > 97% in the H2O solvent system, showing high potential as an industrial catalyst for the AAL epoxidation reaction.","PeriodicalId":381136,"journal":{"name":"Chemical Synthesis","volume":"4 2","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139802498","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Xianchen Gong, Jie Tuo, Jilong Wang, Xintong Li, Chengwei Zhai, Hao Xu, Peng Wu
{"title":"Hydrophilic Ti-MWW for catalyzing epoxidation of allyl alcohol","authors":"Xianchen Gong, Jie Tuo, Jilong Wang, Xintong Li, Chengwei Zhai, Hao Xu, Peng Wu","doi":"10.20517/cs.2023.59","DOIUrl":"https://doi.org/10.20517/cs.2023.59","url":null,"abstract":"Titanosilicates are widely applied in the alkene epoxidation reactions with high reaction rate and selectivity to desired products. Their catalytic performance depends on the structure topology, the micro-environment of Ti active sites, and the hydrophobicity/hydrophilicity of zeolite framework. Herein, we focus on a hydrophilic substrate of allyl alcohol (AAL) and investigated catalytic performance of four titanosilicates (TS-1, Ti-MOR, Ti-MWW, and Re-Ti-MWW) in the AAL epoxidation reaction with hydrogen peroxide as the oxidant. Among them, Re-Ti-MWW, synthesized via the post-modification of Ti-MWW with piperidine, exhibited the highest activity. Moreover, the preferred solvent changed from MeCN for Ti-MWW to H2O for Re-Ti-MWW. The relative diffusion rate of AAL over Re-Ti-MWW was up to 466 × 10-7 s-1, much larger than those of other zeolites. The higher diffusion rate of Re-Ti-MWW was probably derived from the higher framework hydrophilicity as revealed by the smaller water contact angle of Re-Ti-MWW compared to the other zeolites, which contributed to the high activity in AAL epoxidation. In the continuous slurry reactor, Re-Ti-MWW achieved a high catalytic lifetime of 163 h, with the selectivity of desirable glycidol product maintained at > 97% in the H2O solvent system, showing high potential as an industrial catalyst for the AAL epoxidation reaction.","PeriodicalId":381136,"journal":{"name":"Chemical Synthesis","volume":"224 4","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139862498","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Catalyst-free decarboxylative alkylation: access to quaternary center","authors":"Lulan Cai, Fang Li, Shuting Wang, Wentao Xu","doi":"10.20517/cs.2023.57","DOIUrl":"https://doi.org/10.20517/cs.2023.57","url":null,"abstract":"The formation of C(sp3)−C(sp3) bonds has received continuous attention in organic synthesis, and the focus on versatile alkyl precursors remains constant. In our work, prevalent amines and carboxylic acids successfully serve as alkyl sources to construct C(sp3)−C(sp3) bonds via decarboxylative deamination. The catalyst-free decarboxylative alkylation reaction provides alternative access to the quaternary center. Primary mechanistic experiments suggest that it undergoes a polar mechanism.","PeriodicalId":381136,"journal":{"name":"Chemical Synthesis","volume":" 457","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139617953","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Le Liu, Xintian Su, Meiling Qi, Xinyue Gao, Hao Ren, Long Chen
{"title":"Facile synthesis of heteroporous covalent organic frameworks with dual linkages: a “three-in-one” strategy","authors":"Le Liu, Xintian Su, Meiling Qi, Xinyue Gao, Hao Ren, Long Chen","doi":"10.20517/cs.2023.51","DOIUrl":"https://doi.org/10.20517/cs.2023.51","url":null,"abstract":"Covalent organic frameworks (COFs) with dual linkages can combine advantages and properties of two distinct connectors, enabling the development of multifunctional materials. However, due to challenges in simultaneously forming two types of linkages, the synthesis of COFs with dual linkages remains a significant challenge. Herein, we propose a “three-in-one” molecular design strategy for synthesizing COFs with dual linkages (4-amino-4\"-(2,2-dioxan-1,3-dioxan-5-yl)-[1,1':3',1\"-terphenyl]-5'-yl) boronic acid (ADTB)-COF and (4'-amino-5'-(4-(2,2-dioxan-1,3-dioxan-5-yl)phenyl)-[1,1':3',1'-teroxan]-5-yl) boronic acid (ADPB)-COF through reversible condensation between three distinct functionalization groups on the monomer. Benefitting from the abundant micropores and high surface area, ADPB-COF showed excellent selective adsorption capability of C3H8 over CH4 (174, 298 K/1 bar). The present work introduces a new approach for constructing COFs with dual linkages, which greatly simplifies the synthesis process and provides a novel opportunity to develop functional materials based on COFs with multi-linkages.","PeriodicalId":381136,"journal":{"name":"Chemical Synthesis","volume":"3 5","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139529240","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Dan Wen, Saikat Das, Yu Zhao, Jingru Fu, Zelong Qiao, Yijing Gao, Yuxia Wang, Ziqiang Zhao, Dapeng Cao, Daoling Peng, Weidong Zhu, Teng Ben
{"title":"Catalyst-free solid-state cross-linking of covalent organic frameworks in confined space","authors":"Dan Wen, Saikat Das, Yu Zhao, Jingru Fu, Zelong Qiao, Yijing Gao, Yuxia Wang, Ziqiang Zhao, Dapeng Cao, Daoling Peng, Weidong Zhu, Teng Ben","doi":"10.20517/cs.2023.45","DOIUrl":"https://doi.org/10.20517/cs.2023.45","url":null,"abstract":"A “confined space” provides a unique environment to regulate the crystallization thermodynamics and kinetics by confining the reactants in the restricted space dimensions. Solid-state crystal-to-crystal transitions in confined space are controlled by the preassembly of molecules in a crystal lattice and occur inside the lattice. Herein, we report the first case of construction of crystalline cross-linked covalent organic frameworks (CL-COFs) through solid-state cross-linking of acetylenic groups-bridged 2D COFs in spatially limited systems. Specifically, this transformation is thermally induced, yielding CL-COFs with superlative properties, including outstanding enhancement in crystallinity, specific surface area, and stability. We further demonstrate the CL-COFs as high conductivity polymers after iodine doping. This work underscores the opportunity to use lattice-constrained solid-state cross-linking to develop more versatile and feature-rich polyacetylene networks.","PeriodicalId":381136,"journal":{"name":"Chemical Synthesis","volume":" 8","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-01-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139624132","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Recent progress of in-situ/operando characterization approaches of zinc-air batteries","authors":"Jian-Feng Xiong, Mengshi Wang, Ruo-Bei Huang, Jing-Hua Tian, Jian-Feng Li, Zhong-Qun Tian","doi":"10.20517/cs.2023.46","DOIUrl":"https://doi.org/10.20517/cs.2023.46","url":null,"abstract":"Zinc-air batteries (ZABs) belong to the category of metal-air batteries, with high theoretical energy density, safety, and low cost. Nevertheless, there are still many challenges that need to be solved for the practical application of ZABs, including high overpotential, poor cycle life, and so on. This article first briefly introduced the principle of ZABs, covering the key components, functions of each element, and challenges faced by the system. Subsequently, seven methods for studying ZABs in-situ or operando were introduced, including X-ray computed tomography (XCT), optical microscopy imaging (OMI), transmission electron microscopy, nuclear magnetic resonance imaging (MRI), X-ray diffraction (XRD), Raman spectroscopy, and X-ray absorption spectroscopy, accompanied by specific research examples. The future perspectives of ZAB characterization have also been discussed.","PeriodicalId":381136,"journal":{"name":"Chemical Synthesis","volume":" 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2023-12-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139145171","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Dynamic evolution of HZSM-5 zeolite framework under steam treatment","authors":"Lin-Hai He, Jun-Jie Li, Song-Yue Han, Dong Fan, Xiu-Jie Li, Shu-Tao Xu, Ying-Xu Wei, Zhong-Min Liu","doi":"10.20517/cs.2023.55","DOIUrl":"https://doi.org/10.20517/cs.2023.55","url":null,"abstract":"Understanding the dynamic evolution of zeolite framework structures and the interactions between various hydroxyl groups or aluminum species under different steam conditions at the atomic scale is extremely crucial. Herein, using a series of characterization methods, the framework structures of HZSM-5 zeolites (Si/Al = 36) following exposure to steam in the temperature range of 100 to 500 °C are investigated. Under mild steam conditions (T ≤ 200 °C), dealumination is nearly absent, and the silanol nests directly condense to create new framework Si-O-Si bonds. Conversely, under severe steam conditions (T ≥ 300 °C), the framework tetrahedral aluminum atoms Al(IV)-1 can be sequentially converted to partially coordinated framework aluminum Al(IV)-2 and extra-framework aluminum (EFAL) through partial and complete hydrolysis, which cause an increase in the framework Si/Al ratio and a decrease in crystallinity. Al(IV)-2 is recognized as a significant intermediate species for framework complete dealumination. The Brønsted acid sites on Al(IV)-2 can be perturbed by the framework Al-OH groups due to hydrogen bonding interactions, leading to a shift in 1H chemical shifts to lower fields, appearing at 6.0-9.0 ppm and 12.0-15.0 ppm. The newly generated EFAL and silanol nests further evolve through condensation as well. Meanwhile, during dealumination, the spatial correlations (or interactions) of various hydroxyl groups on structurally distinct aluminum species [Al(IV)-1, Al(IV)-2, and EFAL] and aluminum species become extremely intricate. Based on these findings, the dynamic evolution path of HZSM-5 zeolite framework structures under mild and severe steam conditions is proposed.","PeriodicalId":381136,"journal":{"name":"Chemical Synthesis","volume":"31 3","pages":""},"PeriodicalIF":0.0,"publicationDate":"2023-12-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139148212","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Glucose photorefinery for sustainable hydrogen and value-added chemicals coproduction","authors":"Zhe Sun, Heng Zhao, Xinti Yu, Jinguang Hu, Zhangxin Chen","doi":"10.20517/cs.2023.41","DOIUrl":"https://doi.org/10.20517/cs.2023.41","url":null,"abstract":"As a naturally occurring and stable energy supply, biomass will be the leading renewable energy in the future, and its high-value application will help promote the realization of carbon neutrality. Glucose, as the basic unit of lignocellulosic biomass, has been widely investigated as the feedstock to produce various value-added chemicals. Compared to the traditional glucose valorization platforms, such as thermal catalysis and biological fermentation, solar-driven photocatalysis holds the advantages in mild reaction conditions and controllable reaction kinetics, and it is emerging as a sustainable and efficient technology for glucose conversion. With the rational design of the photocatalysts, glucose could be selectively converted into specified chemicals via oriented bond cleavage along with the sustainable generation of hydrogen at the same time, which is the so-called glucose photorefinery process. This present review introduces the general principles and latest progress in glucose photorefinery. The rational design of bifunctional photocatalysts to achieve extended light absorption, efficient charge separation, and favorable surface reaction is also introduced. The oriented breakage of the chemical bonds in glucose molecules to produce different chemicals on different active sites is highlighted. Finally, challenges and perspectives on glucose photorefinery to achieve further efficiency and more fruitful reaction pathways are proposed. This present review is believed to provide guidance for the biomass valorization by mild photocatalysis to simultaneously produce sustainable fuels and chemicals with the rational design of dually functional photocatalysts.","PeriodicalId":381136,"journal":{"name":"Chemical Synthesis","volume":"107 41","pages":""},"PeriodicalIF":0.0,"publicationDate":"2023-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138958740","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Prof. Alain Krief, a brilliant scientist, a passionate chemist and a fantastic chemist trainer","authors":"Bao-Lian Su","doi":"10.20517/cs.2023.62","DOIUrl":"https://doi.org/10.20517/cs.2023.62","url":null,"abstract":"","PeriodicalId":381136,"journal":{"name":"Chemical Synthesis","volume":"56 9","pages":""},"PeriodicalIF":0.0,"publicationDate":"2023-12-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138596724","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}