{"title":"Direct observation of natural products bound to protein based on UHPLC-ESI-MS combined with molecular dynamics simulation","authors":"Jinqi Yang, Xiaoxian Hu, Yuanyuan Zhang, Lingyu Zhao, Chunlin Yue, Yuan Cao, Yangyang Zhang, Zhenwen Zhao","doi":"10.1016/j.cclet.2024.110128","DOIUrl":"https://doi.org/10.1016/j.cclet.2024.110128","url":null,"abstract":"","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":null,"pages":null},"PeriodicalIF":9.1,"publicationDate":"2024-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141393532","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}
Pub Date : 2024-05-31DOI: 10.1016/j.cclet.2024.110060
Wenlong Li , Feishi Shan , Qingdong Bao , Qinghua Li , Hua Gao , Leyong Wang
{"title":"Supramolecular assembly nanoparticle for trans-epithelial treatment of keratoconus","authors":"Wenlong Li , Feishi Shan , Qingdong Bao , Qinghua Li , Hua Gao , Leyong Wang","doi":"10.1016/j.cclet.2024.110060","DOIUrl":"https://doi.org/10.1016/j.cclet.2024.110060","url":null,"abstract":"","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-05-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141541880","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}
Pub Date : 2024-05-31DOI: 10.1016/j.cclet.2024.110074
Two o-carborane based tetraphenylethene (TPE) cationic cyclophanes O1·4PF6 and O2·4PF6 were synthesized through an SN2 reaction. Their structures were confirmed both possessing Z-shaped cavities in single crystal analysis. The optical properties of these macrocycles were systematically investigated using UV–vis spectroscopy and fluorescence techniques. It is worth noting that the introduction of a methoxy group to the TPE unit enables the synthesis of a near-infrared-emitting macrocycle O2·4PF6. The recognition behaviors of these two macrocycles towards nucleotides were investigated using various techniques including fluorescence titration, UV–vis titration, and transmission electron microscopy (TEM). Interestingly, these cyclophanes exhibited aggregation-induced emission (AIE) effects in water or under the induction of nucleotides.
{"title":"Synthesis and properties of tetraphenylethene cationic cyclophanes based on o-carborane skeleton","authors":"","doi":"10.1016/j.cclet.2024.110074","DOIUrl":"10.1016/j.cclet.2024.110074","url":null,"abstract":"<div><p>Two <em>o</em>-carborane based tetraphenylethene (TPE) cationic cyclophanes <strong>O1·4PF<sub>6</sub></strong> and <strong>O2·4PF<sub>6</sub></strong> were synthesized through an S<sub>N</sub>2 reaction. Their structures were confirmed both possessing Z-shaped cavities in single crystal analysis. The optical properties of these macrocycles were systematically investigated using UV–vis spectroscopy and fluorescence techniques. It is worth noting that the introduction of a methoxy group to the TPE unit enables the synthesis of a near-infrared-emitting macrocycle <strong>O2·4PF<sub>6</sub></strong>. The recognition behaviors of these two macrocycles towards nucleotides were investigated using various techniques including fluorescence titration, UV–vis titration, and transmission electron microscopy (TEM). Interestingly, these cyclophanes exhibited aggregation-induced emission (AIE) effects in water or under the induction of nucleotides.</p></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-05-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142097423","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}
Pub Date : 2024-05-29DOI: 10.1016/j.cclet.2024.110068
The rational design of high-performance bifunctional electrocatalysts for overall water splitting (OWS) is the key to popularize hydrogen production technology. The active metal oxyhydroxide (MOOH) formed after surface self-reconfiguration of transition metal sulfide (TMS) electrocatalyst is often regarded as the "actual catalyst" in oxygen evolution reaction (OER). Herein, an Fe doped CoS2/MoS2 hollow TMS polyhedron (Fe-CoS2/MoS2) with rich Mott-Schottky heterojunction is reported and directly utilized as an OWS electrocatalyst. The spontaneous built-in electric field (BEF) at the heterogeneous interface regulates the electronic structure and D-band center of the catalyst. More importantly, the “TMS-MOOH” core-shell structure obtained in the KOH electrolyte shows enhanced OER properties. And the introduction of Fe ions activates the inert basal plane of MoS2, which greatly steps up the performance of HER. Hence, the preferable Fe-CoS2/MoS2–400 presents superior OER activity (η10 = 178 mV, η100 = 375 mV), HER activity (η10 = 92 mV) and ultra-high stability for 50 h. This work has deeply explored the catalytic mechanism of TMS and provided a new idea for the construction of efficient bifunctional catalysts.
合理设计用于整体水分离(OWS)的高性能双功能电催化剂是推广制氢技术的关键。过渡金属硫化物(TMS)电催化剂表面自重构后形成的活性金属氧氢氧化物(MOOH)通常被视为氧进化反应(OER)中的 "实际催化剂"。本文报告了一种具有丰富莫特-肖特基异质结的掺铁 CoS2/MoS2 空心 TMS 多面体(Fe-CoS2/MoS2),并将其直接用作 OWS 电催化剂。异质界面上的自发内置电场(BEF)调节了催化剂的电子结构和 D 波段中心。更重要的是,在 KOH 电解质中获得的 "TMS-MOOH "核壳结构显示出更强的 OER 性能。铁离子的引入激活了 MoS2 的惰性基面,从而大大提高了 HER 的性能。因此,优选的 Fe-CoS2/MoS2-400 具有优异的 OER 活性(η10 = 178 mV,η100 = 375 mV)、HER 活性(η10 = 92 mV)和 50 h 的超高稳定性。这项工作深入探讨了 TMS 的催化机理,为构建高效的双功能催化剂提供了新思路。
{"title":"Built-in electric field and core-shell structure of the reconstructed sulfide heterojunction accelerated water splitting","authors":"","doi":"10.1016/j.cclet.2024.110068","DOIUrl":"10.1016/j.cclet.2024.110068","url":null,"abstract":"<div><p>The rational design of high-performance bifunctional electrocatalysts for overall water splitting (OWS) is the key to popularize hydrogen production technology. The active metal oxyhydroxide (MOOH) formed after surface self-reconfiguration of transition metal sulfide (TMS) electrocatalyst is often regarded as the \"actual catalyst\" in oxygen evolution reaction (OER). Herein, an Fe doped CoS<sub>2</sub>/MoS<sub>2</sub> hollow TMS polyhedron (Fe-CoS<sub>2</sub>/MoS<sub>2</sub>) with rich Mott-Schottky heterojunction is reported and directly utilized as an OWS electrocatalyst. The spontaneous built-in electric field (BEF) at the heterogeneous interface regulates the electronic structure and D-band center of the catalyst. More importantly, the “TMS-MOOH” core-shell structure obtained in the KOH electrolyte shows enhanced OER properties. And the introduction of Fe ions activates the inert basal plane of MoS<sub>2</sub>, which greatly steps up the performance of HER. Hence, the preferable Fe-CoS<sub>2</sub>/MoS<sub>2</sub>–400 presents superior OER activity (<em>η</em><sub>10</sub> = 178 mV, <em>η</em><sub>100</sub> = 375 mV), HER activity (<em>η</em><sub>10</sub> = 92 mV) and ultra-high stability for 50 h. This work has deeply explored the catalytic mechanism of TMS and provided a new idea for the construction of efficient bifunctional catalysts.</p></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-05-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142149304","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}
Pub Date : 2024-05-28DOI: 10.1016/j.cclet.2024.110050
Benzo[4,5]imidazo[1,2-a]pyrimidine-based derivatives play crucial roles in medicines, pesticides, tracers and photoelectric materials. However, their synthesis approach still needs to be optimized, and their fluorescent properties in intracellular microenvironment are unclear. Here, a Cu(II)-catalyzed cascade coupling cyclization reaction was successfully developed to synthesize benzo[4,5]imidazo[1,2-a]pyrimidine scaffold with mild reaction conditions, broad substrate scopes and high yields. After a system study, we found that compound 4aa displayed an optimal viscosity-specific response with remarkable fluorescence enhancement (102-fold) for glycerol at 490 nm. Particularly, 4aa possessed excellent structure-inherent targeting (SIT) capability for lysosome (P = 0.95) with high pH stability and large Stokes shift. Importantly, 4aa was validated for its effectiveness in diagnosing lysosomal storage disorders (LSD) in living cells. The 4aa also showed its potential to map the micro-viscosity and its metabolism process in zebrafish. This work not only affords an efficient protocol to fabricate benzo[4,5]imidazo[1,2-a]pyrimidine derivatives, reveals this skeleton has excellent SIT features for lysosome, but also manifests that 4aa can serve as a practical tool to monitor lysosomal viscosity and diagnose LSD.
{"title":"Benzo[4,5]imidazo[1,2-a]pyrimidine-based structure-inherent targeting fluorescent sensor for imaging lysosomal viscosity and diagnosis of lysosomal storage disorders","authors":"","doi":"10.1016/j.cclet.2024.110050","DOIUrl":"10.1016/j.cclet.2024.110050","url":null,"abstract":"<div><p>Benzo[4,5]imidazo[1,2-<em>a</em>]pyrimidine-based derivatives play crucial roles in medicines, pesticides, tracers and photoelectric materials. However, their synthesis approach still needs to be optimized, and their fluorescent properties in intracellular microenvironment are unclear. Here, a Cu(II)-catalyzed cascade coupling cyclization reaction was successfully developed to synthesize benzo[4,5]imidazo[1,2-<em>a</em>]pyrimidine scaffold with mild reaction conditions, broad substrate scopes and high yields. After a system study, we found that compound <strong>4aa</strong> displayed an optimal viscosity-specific response with remarkable fluorescence enhancement (102-fold) for glycerol at 490 nm. Particularly, <strong>4aa</strong> possessed excellent structure-inherent targeting (SIT) capability for lysosome (<em>P</em> = 0.95) with high pH stability and large Stokes shift. Importantly, <strong>4aa</strong> was validated for its effectiveness in diagnosing lysosomal storage disorders (LSD) in living cells. The <strong>4aa</strong> also showed its potential to map the micro-viscosity and its metabolism process in zebrafish. This work not only affords an efficient protocol to fabricate benzo[4,5]imidazo[1,2-<em>a</em>]pyrimidine derivatives, reveals this skeleton has excellent SIT features for lysosome, but also manifests that <strong>4aa</strong> can serve as a practical tool to monitor lysosomal viscosity and diagnose LSD.</p></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-05-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141935168","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}
Pub Date : 2024-05-28DOI: 10.1016/j.cclet.2024.110061
Fengyao Cui , Qiaona Zhang , Tangxin Xiao , Zhouyu Wang , Leyong Wang
{"title":"Reversible phosphorescence in pseudopolyrotaxane elastomer","authors":"Fengyao Cui , Qiaona Zhang , Tangxin Xiao , Zhouyu Wang , Leyong Wang","doi":"10.1016/j.cclet.2024.110061","DOIUrl":"https://doi.org/10.1016/j.cclet.2024.110061","url":null,"abstract":"","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-05-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141481842","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}
An efficient and scalable electrochemical asymmetric protocol with metal-free catalysts and even without additional oxidants for the cross-dehydrogenative coupling reaction (CDC) of two C(sp3)-H bonds is reported. A series of aldehydes including natural products and various substrates containing C(sp3)-H bonds including xanthenes, acridines, cycloheptatrienes and even diarylmethane have been shown to undergo asymmetric CDC to afford a series of carbon-carbon bond coupling products with up to 94% yield and 98% ee. Mechanistic studies such as radical clock experiment suggest that the reaction proceeds via nucleophilic attack by enamine under electrochemical conditions.
{"title":"Electricity-driven enantioselective cross-dehydrogenative coupling of two C(sp3)-H bonds enabled by organocatalysis","authors":"Yuemin Chen, Yunqi Wu, Guoao Wang, Feihu Cui, Haitao Tang, Yingming Pan","doi":"10.1016/j.cclet.2023.109445","DOIUrl":"https://doi.org/10.1016/j.cclet.2023.109445","url":null,"abstract":"<div><p>An efficient and scalable electrochemical asymmetric protocol with metal-free catalysts and even without additional oxidants for the cross-dehydrogenative coupling reaction (CDC) of two C(sp<sup>3</sup>)-H bonds is reported. A series of aldehydes including natural products and various substrates containing C(sp<sup>3</sup>)-H bonds including xanthenes, acridines, cycloheptatrienes and even diarylmethane have been shown to undergo asymmetric CDC to afford a series of carbon-carbon bond coupling products with up to 94% yield and 98% <em>ee</em>. Mechanistic studies such as radical clock experiment suggest that the reaction proceeds <em>via</em> nucleophilic attack by enamine under electrochemical conditions.</p></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":null,"pages":null},"PeriodicalIF":9.1,"publicationDate":"2024-05-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141163332","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}
Pub Date : 2024-05-27DOI: 10.1016/j.cclet.2024.110055
Surface chemistry focuses on the investigation of the adsorption, migration, assembly, activation, reaction, and desorption of atoms and molecules at surfaces. Surface chemistry plays the pivotal roles in both fundamental science and applied technology. This review will summarize the recent progresses on surface assembly, synthesis and catalysis investigated mainly by scanning tunneling microscopy and atomic force microscopy. Surface assemblies of water and small biomolecules, construction of Sierpiński triangles and surface chirality are summarized. On-surface synthesis of conjugated carbo- and heterocycles and other kinds of carbon nanostructures are surveyed. Surface model catalysis, including single-atom catalysis and electrochemical catalysis, are discussed at the single-atom level.
{"title":"Recent progress on surface chemistry I: Assembly and reaction","authors":"","doi":"10.1016/j.cclet.2024.110055","DOIUrl":"10.1016/j.cclet.2024.110055","url":null,"abstract":"<div><p>Surface chemistry focuses on the investigation of the adsorption, migration, assembly, activation, reaction, and desorption of atoms and molecules at surfaces. Surface chemistry plays the pivotal roles in both fundamental science and applied technology. This review will summarize the recent progresses on surface assembly, synthesis and catalysis investigated mainly by scanning tunneling microscopy and atomic force microscopy. Surface assemblies of water and small biomolecules, construction of Sierpiński triangles and surface chirality are summarized. On-surface synthesis of conjugated carbo- and heterocycles and other kinds of carbon nanostructures are surveyed. Surface model catalysis, including single-atom catalysis and electrochemical catalysis, are discussed at the single-atom level.</p></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-05-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142122403","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}
Pub Date : 2024-05-22DOI: 10.1016/j.cclet.2024.110038
Wen-Tao Ouyang , Jun Jiang , Yan-Fang Jiang , Ting Li , Yuan-Yuan Liu , Hong-Tao Ji , Li-Juan Ou , Wei-Min He
The first example of sono-photocatalytic bond formation was reported. With both visible light and ultrasound wave as the energy, various 3-aminoquinoxalin-2(1H)-ones were efficiently obtained with good functional group tolerance in the absence of any additive or external photocatalyst. Compared with the conventional photocatalysis, sono-photocatalysis not only dramatically improved the reaction rates and yields, but also reduced energy consumption.
{"title":"Sono-photocatalytic amination of quinoxalin-2(1H)-ones with aliphatic amines","authors":"Wen-Tao Ouyang , Jun Jiang , Yan-Fang Jiang , Ting Li , Yuan-Yuan Liu , Hong-Tao Ji , Li-Juan Ou , Wei-Min He","doi":"10.1016/j.cclet.2024.110038","DOIUrl":"10.1016/j.cclet.2024.110038","url":null,"abstract":"<div><p>The first example of sono-photocatalytic bond formation was reported. With both visible light and ultrasound wave as the energy, various 3-aminoquinoxalin-2(1<em>H</em>)-ones were efficiently obtained with good functional group tolerance in the absence of any additive or external photocatalyst. Compared with the conventional photocatalysis, sono-photocatalysis not only dramatically improved the reaction rates and yields, but also reduced energy consumption.</p></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141140228","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}
Pub Date : 2024-05-20DOI: 10.1016/j.cclet.2024.110031
Carbon-based materials with single-atom (SA) transition metals coordinated with nitrogen (M-Nx) have attracted extensive attention due to their superior electrochemical CO2 reduction reaction (CO2RR) performance. However, the uncontrolled recombination of metal atoms during the typical high-temperature synthesis process in M-Nx causes deterioration of CO2RR activity. Herein, by using electrospinning, we propose a novel strategy for constructing a highly active and selective SA Fe-modified N-doped porous carbon fiber membrane catalyst (Fe-N-CF). This carbon membrane has an interconnected three-dimensional structure and a hierarchical porous structure, which can not only confine Fe to be single atom as active centers, but also provide a diffusion channel for CO2 molecules. Relying on its special structure and stable mechanical properties, Fe-N-CF is directly used for CO2RR, which presents an excellent selectivity (CO Faradaic efficiency of 97 %) and stability. DFT calculations reveals that the synthesized Fe-N4-C can significantly reduce the energy barrier for intermediate COOH* formation and CO desorption. This work highlights the specific advantages of using electrospinning method to prepare the optimal SA catalysts.
含有与氮配位的单原子(SA)过渡金属(M-Nx)的碳基材料因其卓越的电化学二氧化碳还原反应(CO2RR)性能而受到广泛关注。然而,在 M-Nx 典型的高温合成过程中,金属原子的不可控重组会导致 CO2RR 活性下降。在此,我们提出了一种利用电纺丝技术构建高活性和高选择性 SA Fe 改性 N 掺杂多孔碳纤维膜催化剂(Fe-N-CF)的新策略。这种碳膜具有相互连接的三维结构和分层多孔结构,不仅能将铁限制为单个原子作为活性中心,还能为二氧化碳分子提供扩散通道。凭借其特殊的结构和稳定的力学性能,Fe-N-CF 被直接用于 CO2RR,具有极佳的选择性(CO 法拉效率达 97%)和稳定性。DFT 计算显示,合成的 Fe-N4-C 能显著降低中间 COOH* 形成和 CO 解吸的能障。这项工作凸显了使用电纺丝方法制备最佳 SA 催化剂的具体优势。
{"title":"Coordination-based synthesis of Fe single-atom anchored nitrogen-doped carbon nanofibrous membrane for CO2 electroreduction with nearly 100 % CO selectivity","authors":"","doi":"10.1016/j.cclet.2024.110031","DOIUrl":"10.1016/j.cclet.2024.110031","url":null,"abstract":"<div><p>Carbon-based materials with single-atom (SA) transition metals coordinated with nitrogen (M-N<sub>x</sub>) have attracted extensive attention due to their superior electrochemical CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) performance. However, the uncontrolled recombination of metal atoms during the typical high-temperature synthesis process in M-N<sub>x</sub> causes deterioration of CO<sub>2</sub>RR activity. Herein, by using electrospinning, we propose a novel strategy for constructing a highly active and selective SA Fe-modified N-doped porous carbon fiber membrane catalyst (Fe-N-CF). This carbon membrane has an interconnected three-dimensional structure and a hierarchical porous structure, which can not only confine Fe to be single atom as active centers, but also provide a diffusion channel for CO<sub>2</sub> molecules. Relying on its special structure and stable mechanical properties, Fe-N-CF is directly used for CO<sub>2</sub>RR, which presents an excellent selectivity (CO Faradaic efficiency of 97 %) and stability. DFT calculations reveals that the synthesized Fe-N<sub>4</sub>-C can significantly reduce the energy barrier for intermediate COOH* formation and CO desorption. This work highlights the specific advantages of using electrospinning method to prepare the optimal SA catalysts.</p></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-05-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141145374","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}