Chemical Synthesis最新文献

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Immobilized enzymatic alcohol oxidation as a versatile reaction module for multienzyme cascades 作为多酶级联多功能反应模块的固定化酶解酒精氧化技术
Chemical Synthesis Pub Date : 2023-11-27 DOI: 10.20517/cs.2023.40
Kesheng Fu, Lele Dong, Pengbo Liu, Li-Yi Zhou, Guanhua Liu, Jing Gao, Bingjun Gao, Yunting Liu, Yanjun Jiang
{"title":"Immobilized enzymatic alcohol oxidation as a versatile reaction module for multienzyme cascades","authors":"Kesheng Fu, Lele Dong, Pengbo Liu, Li-Yi Zhou, Guanhua Liu, Jing Gao, Bingjun Gao, Yunting Liu, Yanjun Jiang","doi":"10.20517/cs.2023.40","DOIUrl":"https://doi.org/10.20517/cs.2023.40","url":null,"abstract":"Enzymatic alcohol oxidation (EAO) is highly attractive thanks to its efficiency, selectivity, and sustainability benefits, but it is often neglected as a catalytic tool for practical production due to the instability and non-reusability of enzymes. Herein, a non-enantioselective alcohol dehydrogenase engineered from Candida parapsilosis (Cps ADH) and a laccase from Trametes versicolor was immobilized on mesoporous silica nanoflowers (MSNs), fabricating Cps ADH@MSNs (41 U/gsupport) and laccase@MSNs (67 U/gsupport) for EAO, respectively. The structural and functional properties of the MSNs endowed the immobilized enzymes with higher stability than free enzymes, and the relative activity of the immobilized enzyme was 52% and 63%, respectively, after being reused five times. The immobilized enzymes exhibited high activity, selectivity, and complementary substrate specificity in alcohol oxidation. The optimized EAO, as a versatile cascade module, was coupled with several other enzymatic transformations for multi-enzymatic synthesis of high value-added chemicals. The chiral alcohols and amines were produced with 99% ee and 84% to 98% ee, respectively, and (R )-benzoin and 2-furoic acid were prepared with 91% yield, 99% ee and 86% yield, respectively, demonstrating the synthetic utility of the immobilized enzymes.","PeriodicalId":381136,"journal":{"name":"Chemical Synthesis","volume":"16 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2023-11-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139232558","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}
引用次数: 0
Proton exchange membrane fuel cells: application for value-added chemical productions 质子交换膜燃料电池:应用于增值化学品生产
Chemical Synthesis Pub Date : 2023-11-27 DOI: 10.20517/cs.2023.44
Xia Jiang, Rui Chen, Yanxin Chen, Canggui Lu
{"title":"Proton exchange membrane fuel cells: application for value-added chemical productions","authors":"Xia Jiang, Rui Chen, Yanxin Chen, Canggui Lu","doi":"10.20517/cs.2023.44","DOIUrl":"https://doi.org/10.20517/cs.2023.44","url":null,"abstract":"Proton exchange membrane fuel cells (PEMFCs) can be used as reactors to produce chemicals and co-generate electricity and chemicals. Their mild reaction conditions, high product selectivity, and energy utilization have profoundly impacted gas separation, water treatment, and energy utilization fields. Given the lack of systematic reports on the current research status of utilizing PEMFCs for chemical production and the co-production of electricity and chemicals, this article summarizes the types of reactions and catalyst usage involved in this multifaceted application. It analyzes how to improve the production and performance of the system from four aspects: electrolyte membranes, catalysts, assembly methods, and reaction processes. Finally, the article analyzes the current research shortcomings in utilizing PEMFCs for these applications and provides prospects for future development.","PeriodicalId":381136,"journal":{"name":"Chemical Synthesis","volume":"9 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2023-11-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139233606","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}
引用次数: 0
A comparative study between Monte Carlo entropic sampling method and local mean field investigations of thermal properties of spin-crossover nanoparticles based on Ising-like model 基于 Ising-like 模型的蒙特卡罗熵采样法与自旋交叉纳米粒子热特性的局部均值场研究对比研究
Chemical Synthesis Pub Date : 2023-11-18 DOI: 10.20517/cs.2023.23
J. Linares, C. Cazelles, Pierre Richard Dahoo, N. Belmouri, K. Boukheddaden
{"title":"A comparative study between Monte Carlo entropic sampling method and local mean field investigations of thermal properties of spin-crossover nanoparticles based on Ising-like model","authors":"J. Linares, C. Cazelles, Pierre Richard Dahoo, N. Belmouri, K. Boukheddaden","doi":"10.20517/cs.2023.23","DOIUrl":"https://doi.org/10.20517/cs.2023.23","url":null,"abstract":"The thermally induced transitions between low-spin (LS) and high-spin (HS) configurations of spin-crossover (SCO) nanoparticles are simulated, focusing on the effects of localized surface and bulk interactions on the average magnetization of 2D square lattices. The thermal behaviors and hysteresis cycles are investigated within the framework of the Ising model Hamiltonian and are conducted following two approaches: local mean field approximation (LMFA) and Monte Carlo entropic sampling (MCES) techniques. The results obtained by these two methods are compared for the two square lattice sizes, 6 $$ times $$ 6 and 7 $$ times $$ 7. Thus, when the bulk-surface interaction term is set to zero, the two approaches lead to identical values of the surface and bulk transition temperatures separated by a long intermediate plateau in both cases. Although hysteresis curves exhibit a similar shape, LMFA shows slightly larger widths $$ Delta T $$ than MCES. On increasing bulk-surface interaction term, the two methods lead to different shifts in equilibrium temperature values for both bulk and surface components, respectively, to lower and higher values by MCES. In general, it is found that LMFA shifts surface equilibrium temperature differently to lower values and enhances the hysteresis effect, particularly for surface molecules. On the other hand, for the 7 $$ times $$ 7 square lattice, the equilibrium temperatures are slightly higher by 1.5% and 3.2% for bulk and surface molecules, respectively, with a narrower hysteresis width in the surface. Moreover, with the MCES method, an abrupt transition instead of a hysteresis transition is calculated for surface molecules ($$ Delta T_{surf}^{MCES}=0 $$ K).","PeriodicalId":381136,"journal":{"name":"Chemical Synthesis","volume":"7 4","pages":""},"PeriodicalIF":0.0,"publicationDate":"2023-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139261857","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}
引用次数: 0
Dual visible-light and NHC-catalyzed radical relay trifunctionalization of unactivated alkenes 未活化烯烃的可见光和 NHC 双催化自由基中继三官能化
Chemical Synthesis Pub Date : 2023-11-17 DOI: 10.20517/cs.2023.43
Jian-Quan Feng, Luning Li, Jingyi Wang, Aoting Ni, Zexuan Wei, Ding Du, Jie Feng
{"title":"Dual visible-light and NHC-catalyzed radical relay trifunctionalization of unactivated alkenes","authors":"Jian-Quan Feng, Luning Li, Jingyi Wang, Aoting Ni, Zexuan Wei, Ding Du, Jie Feng","doi":"10.20517/cs.2023.43","DOIUrl":"https://doi.org/10.20517/cs.2023.43","url":null,"abstract":"Radical trifunctionalization of unactivated alkenes remains rare and challenging, although they can provide a robust tool for the construction of molecules with high added value from simple materials. This work presents the relay dual N-heterocyclic carbene organocatalytic and visible-light photocatalytic multi-component trifunctionalization of alkyl alkenes via the merger of remote 1,4-cyano migration and alkylacylation. The method features a broad substrate scope and good compatibility of diverse functional groups. Density functional theory calculations were also carried out to rationalize the origin of this reaction. The cooperative N-heterocyclic carbene and photoredox catalysis enabled reductive single-electron transfer reaction of acyl azolium species and subsequent radical-radical cross-coupling, allowing for the facile construction of three new C−C bonds in one-pot reactions with high regioselectivity.","PeriodicalId":381136,"journal":{"name":"Chemical Synthesis","volume":"41 3","pages":""},"PeriodicalIF":0.0,"publicationDate":"2023-11-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139264558","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}
引用次数: 0
Strain engineering of two-dimensional materials for energy storage and conversion applications 用于能量存储和转换应用的二维材料应变工程
Chemical Synthesis Pub Date : 2023-11-03 DOI: 10.20517/cs.2023.34
Xing Peng, Long Chen, Yifan Liu, Chao Liu, Honglan Huang, Jinbo Fan, Pan Xiong, Junwu Zhu
{"title":"Strain engineering of two-dimensional materials for energy storage and conversion applications","authors":"Xing Peng, Long Chen, Yifan Liu, Chao Liu, Honglan Huang, Jinbo Fan, Pan Xiong, Junwu Zhu","doi":"10.20517/cs.2023.34","DOIUrl":"https://doi.org/10.20517/cs.2023.34","url":null,"abstract":"Two-dimensional (2D) materials have garnered much interest due to their exceptional optical, electrical, and mechanical properties. Strain engineering, as a crucial approach to modulate the physicochemical characteristics of 2D materials, has been widely used in various fields, especially for energy storage and conversion. Herein, the recent progress in strain engineering of 2D materials is summarized for energy storage and conversion applications. The fundamental understanding of strain in 2D materials is first described. Then, some synthetic methods for modulating the properties of 2D materials via strain engineering are introduced. Further, the applications of strain engineering of 2D materials in energy storage, photocatalysis, and electrocatalysis are discussed. Finally, the challenges and perspectives on strain engineering of 2D materials are also outlined.","PeriodicalId":381136,"journal":{"name":"Chemical Synthesis","volume":"12 7","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-11-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135869123","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}
引用次数: 0
The synthesis, characterization and application of the binol-cages of R-/S-enantiomers R-/ s对映体双醇笼的合成、表征及应用
Chemical Synthesis Pub Date : 2023-10-31 DOI: 10.20517/cs.2023.39
Tianyu Li, Luyao Ding, Yihong Kang, Xin-Qi Hao, Yujing Guo, Linlin Shi, Mao-Ping Song
{"title":"The synthesis, characterization and application of the binol-cages of R-/S-enantiomers","authors":"Tianyu Li, Luyao Ding, Yihong Kang, Xin-Qi Hao, Yujing Guo, Linlin Shi, Mao-Ping Song","doi":"10.20517/cs.2023.39","DOIUrl":"https://doi.org/10.20517/cs.2023.39","url":null,"abstract":"In the past few years, significant efforts have been made to create and self-assemble covalent organic cages with increased complexity and functionality. However, although supramolecule cages have been widely recognized as probes to identify metal ions, the detection of mercury ions has not been fully developed. Here, we have designed and synthesized a pair of chiral cages with custom cavities based on the unique rigid structure of 1, 10-binaphthol (binol). Meanwhile, the supramolecular cage has excellent performance in high sensitivity and selectivity for detecting mercury ions. The UV titration results indicate that the binding ratio of the host to guest is 1:5. The titration curve conforms to the nonlinear fitting of the Hill function, which can obtain the binding constant K = 2.57 × 105 M-1 . Furthermore, the detection limit of 1.9 × 10-7 M can be obtained because the absorbance of cages exhibits a strong linear relationship with Hg2+ concentrations. This work provides a new method for selective recognition of ions by supramolecular cages.","PeriodicalId":381136,"journal":{"name":"Chemical Synthesis","volume":"15 8","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-10-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135808176","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}
引用次数: 0
Energy-efficient anodic reactions for sustainable hydrogen production via water electrolysis 通过水电解实现可持续制氢的节能阳极反应
Chemical Synthesis Pub Date : 2023-10-13 DOI: 10.20517/cs.2023.28
Wenxian Liu, Xinxin Niu, Jiawei Tang, Qian Liu, Jun Luo, Xijun Liu, Yingtang Zhou
{"title":"Energy-efficient anodic reactions for sustainable hydrogen production via water electrolysis","authors":"Wenxian Liu, Xinxin Niu, Jiawei Tang, Qian Liu, Jun Luo, Xijun Liu, Yingtang Zhou","doi":"10.20517/cs.2023.28","DOIUrl":"https://doi.org/10.20517/cs.2023.28","url":null,"abstract":"Overall water splitting is considered as an effective technique for hydrogen (H2) production; however, it usually requires large operating voltage mainly due to the high equilibrium potential of the anodic oxygen evolution reaction (OER). Replacing OER with energy-saving anode reactions not only reduces the operating voltage for H2 production but also generates high-value-added chemicals or purifies wastewater. This review article provides an overview of the fundamental reaction principles of overall water splitting and typical energy-saving alternative anode reactions, including methanol oxidation, hydrazine oxidation, and urea oxidation reactions. Then, the preparation methods, regulation strategies, and composition/structure-performance relations of advanced catalysts for these energy-efficient H2 generation technologies are discussed. Finally, we propose the underlying challenges and perspectives for this promising field.","PeriodicalId":381136,"journal":{"name":"Chemical Synthesis","volume":"16 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-10-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135804928","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}
引用次数: 1
Recent progress of decacarbonyldimanganese catalysis 十羰基二锰催化研究进展
Chemical Synthesis Pub Date : 2023-10-11 DOI: 10.20517/cs.2023.32
Tao Li, Albert S. C. Chan, Shan-Shui Meng
{"title":"Recent progress of decacarbonyldimanganese catalysis","authors":"Tao Li, Albert S. C. Chan, Shan-Shui Meng","doi":"10.20517/cs.2023.32","DOIUrl":"https://doi.org/10.20517/cs.2023.32","url":null,"abstract":"Decacarbonyldimanganese (Mn2(CO)10), one of the most long-standing organometallic reagents, bears a weak Mn-Mn bond, which occurs a homo-cleavage feasibly under heating or light-irritation, delivering an active manganese-centered radical. This highly reactive metallic radical could activate the Si-H bond, C-halogen bond, N-halogen bond, S-halogen bond, and O=O bond, generating corresponding Mn species and Si, C, N, S, and O radicals. This wonderful reactivity enables an extensive utilization of this dimeric manganese in catalytic atom-transfer reactions and oxidation reactions. In this review, we offer a comprehensive review of this growing area in recent decades. Critical comparisons and mechanism analyses are provided, along with personal perspectives for future studies.","PeriodicalId":381136,"journal":{"name":"Chemical Synthesis","volume":"50 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-10-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"136062456","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}
引用次数: 0
Revealing the dynamic formation mechanism of porous Mo2C: an in-situ TEM study 揭示多孔Mo2C的动态形成机制:原位透射电镜研究
Chemical Synthesis Pub Date : 2023-10-10 DOI: 10.20517/cs.2023.33
Yongzhao Wang, Yiming Niu, Yinghui Pu, Shiyan Li, Yuefeng Liu, Bingsen Zhang
{"title":"Revealing the dynamic formation mechanism of porous Mo<sub>2</sub>C: an <i>in-situ</i> TEM study","authors":"Yongzhao Wang, Yiming Niu, Yinghui Pu, Shiyan Li, Yuefeng Liu, Bingsen Zhang","doi":"10.20517/cs.2023.33","DOIUrl":"https://doi.org/10.20517/cs.2023.33","url":null,"abstract":"In-situ transmission electron microscopy (TEM) enables direct observation of the micromorphology and microstructure evolution of catalysts in the chemical atmosphere. Studying the structural evolution during the formation of molybdenum carbide using in-situ TEM is helpful for the preparation of high-performance carbide catalysts. Herein, the formation mechanism of porous Mo2C from MoO2 nanoparticles (NPs) was studied by in-situ TEM. The formation of Mo2C was induced by the defects of MoO2, and the formed Mo2C facilitated the carbonization of neighboring MoO2 NPs. The growth rate of Mo2C between MoO2 NPs was slower compared to that within a single MoO2 NP. In addition, the formation and growth of pores in Mo2C were also studied; the pores grew radially during the early stages from the nucleation sites and later grew branched and curved. As Mo2C underwent competitive growth, the pores transitioned from straight to curved. Eventually, during prolonged carbonization at high temperatures, Mo2C underwent sintering.","PeriodicalId":381136,"journal":{"name":"Chemical Synthesis","volume":"57 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"136296281","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}
引用次数: 0
Recent progress of enhanced bubble separation in alkaline water electrolyzer 碱水电解槽强化气泡分离研究进展
Chemical Synthesis Pub Date : 2023-09-27 DOI: 10.20517/cs.2023.25
Lin Yang, Lingyu Gao, Guixuan Shan, Xinyi Huo, Mengfei Zhang, Yuxuan Wang, Xingyu Liu, Aiqun Kong, Jiangjiexing Wu, Jinli Zhang
{"title":"Recent progress of enhanced bubble separation in alkaline water electrolyzer","authors":"Lin Yang, Lingyu Gao, Guixuan Shan, Xinyi Huo, Mengfei Zhang, Yuxuan Wang, Xingyu Liu, Aiqun Kong, Jiangjiexing Wu, Jinli Zhang","doi":"10.20517/cs.2023.25","DOIUrl":"https://doi.org/10.20517/cs.2023.25","url":null,"abstract":"Alkaline water electrolysis has a large industrial application and development potential in hydrogen energy owing to its high maturity and low cost. However, its moderate energy efficiency, especially caused by bubble effects, inhibits its use for large-scale hydrogen production. To overcome this shortcoming, this review first analyzes the bubble effect and summarizes the external operation methods, such as external field intensification, flow operation, fluctuation operation, and surfactant addition to the electrolyte, to enhance bubble separation in the electrolyzer. Then, electrode and flow channel structure optimization, particularly superhydrophilic and superaerophobic electrodes, and flow channels with varying heights, square column arrangements, and inlet/outlet numbers are highlighted. Finally, future research directions in alkaline water electrolysis technology are suggested to advance the industrial application of large-scale alkaline water electrolysis.","PeriodicalId":381136,"journal":{"name":"Chemical Synthesis","volume":"41 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135537716","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}
引用次数: 0
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