Cailing Wu , Shaojie Wu , Qifei Huang , Kai Sun , Xianqiang Huang , Jianji Wang , Bing Yu
{"title":"Potassium-modified carbon nitride photocatalyzed-aminoacylation of N‑sulfonyl ketimines","authors":"Cailing Wu , Shaojie Wu , Qifei Huang , Kai Sun , Xianqiang Huang , Jianji Wang , Bing Yu","doi":"10.1016/j.cclet.2024.110250","DOIUrl":"10.1016/j.cclet.2024.110250","url":null,"abstract":"<div><div>The development of innovative and sustainable catalytic strategies for organic synthesis is a pivotal aspect of advancing material science and chemical engineering. This research presents a new catalytic method for the aminoacylation of <em>N</em>‑sulfonyl ketimines by utilizing a potassium-doped graphite-like carbon nitride (g-C<sub>3</sub>N<sub>4</sub>) framework. This method not only enhances the catalytic efficiency and broadens the light absorption spectrum of g-C<sub>3</sub>N<sub>4</sub> but also significantly reduces the recombination rate of electron-hole pairs, thereby increasing the reaction yield and selectivity. Importantly, our approach facilitates the synthesis of aminoacylated <em>N</em>-heterocycles, expanding the applicability of potassium-modified g-C<sub>3</sub>N<sub>4</sub> in photocatalytic organic synthesis. A notable accomplishment of this study is the unprecedented generation of carbamoyl radicals <em>via</em> heterogeneous photocatalysis, which can be easily recycled after reaction. This advancement highlights the capability of potassium-doped g-C<sub>3</sub>N<sub>4</sub> (namely <strong>K-CN</strong>) as an advanced heterogeneous photocatalyst for the formation of complex organic compounds.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 2","pages":"Article 110250"},"PeriodicalIF":9.4,"publicationDate":"2024-07-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141846336","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}
Bingke Zhang , Dongbo Wang , Jiamu Cao , Wen He , Gang Liu , Donghao Liu , Chenchen Zhao , Jingwen Pan , Sihang Liu , Weifeng Zhang , Xuan Fang , Liancheng Zhao , Jinzhong Wang
{"title":"Tuning Stark effect by defect engineering on black titanium dioxide mesoporous spheres for enhanced hydrogen evolution","authors":"Bingke Zhang , Dongbo Wang , Jiamu Cao , Wen He , Gang Liu , Donghao Liu , Chenchen Zhao , Jingwen Pan , Sihang Liu , Weifeng Zhang , Xuan Fang , Liancheng Zhao , Jinzhong Wang","doi":"10.1016/j.cclet.2024.110254","DOIUrl":"10.1016/j.cclet.2024.110254","url":null,"abstract":"<div><p>Defects can strongly affect the lattice, strain, and electronic structures of nanomaterials photocatalysts, like a double-edged sword of both positive significance and negative influence on photocatalytic performances. To date, most studies into defects only partially elucidated their beneficial or detrimental roles in photocatalysis. However, a quantitative understanding of the photocatalytic performances modulated by defect concentration still needs to be discovered. Here, a series of TiO<sub>2−</sub><sub>X</sub> mesoporous spheres (MS) with different oxygen vacancy concentrations for photocatalytic applications were prepared by high-temperature chemical reduction. The link between oxygen vacancy concentration and photocatalytic performance was successfully established. The localization of carriers dominated by the Stark effect is first enhanced and then weakened with increasing oxygen vacancy concentration, which is a crucial factor in explaining the double-edged sword role of defect concentration in photocatalysis. As the reduction temperature rises to 300 °C, carrier localization dominated by the quantum-confined Stark effect maximizes the separation ability of photo generated electron hole pairs, thus exhibiting the best catalytic performance for photocatalytic hydrogen production and the degradation of organic pollutants, as demonstrated by a hydrogen evolution rate of 523.7 µmol g<sup>-1</sup> h<sup>-1</sup> and a ninefold higher RhB photodegradation rate compared to TiO<sub>2</sub> MS. The work offers excellent flexibility for precisely constructing high-performance photocatalysts by understanding vacancy engineering.</p></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"35 11","pages":"Article 110254"},"PeriodicalIF":9.4,"publicationDate":"2024-07-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141693719","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":"Chlorination of benzyl group on the terminal unit of A2-A1-D-A1-A2 type nonfullerene acceptor for high-voltage organic solar cells","authors":"Jinge Zhu , Ailing Tang , Leyi Tang , Peiqing Cong , Chao Li , Qing Guo , Zongtao Wang , Xiaoru Xu , Jiang Wu , Erjun Zhou","doi":"10.1016/j.cclet.2024.110233","DOIUrl":"10.1016/j.cclet.2024.110233","url":null,"abstract":"<div><div>Benzotriazole (BTA)-based A<sub>2</sub>-A<sub>1</sub>-D-A<sub>1</sub>-A<sub>2</sub> type wide-bandgap (WBG) non-fullerene acceptors (NFAs) have shown promising potential in indoor photovoltaic, and in-depth investigation of their structure-property relationship is of great significance. Herein, we explored the chlorination effect of the side chain on the terminals. We introduced Cl atoms into the benzyl side chains in parent BTA5 to synthesize two NFAs, BTA5-Cl with mono-chlorinated benzyl groups and BTA5-2Cl containing bi-chlorinated benzyl groups. We chose D18-Cl with deep-energy levels and strong crystallinity to pair with these three acceptors, affording high photovoltage and photocurrent. With the stepwise chlorination, the open-circuit voltage (<em>V</em><sub>OC</sub>) values decrease from 1.28, 1.22, to 1.20 V, while the corresponding power conversion efficiencies (PCEs) improve from 5.07 %, 9.15 %, to 10.96 %. Compared with BTA5-based OSCs, introducing Cl atoms downshifts the energy levels and slightly increases the non-radiative energy loss (0.14 < 0.17 < 0.19 eV), resulting in a sequential decrease in <em>V</em><sub>OC</sub>. However, more chlorine atom replacements produce more effective exciton dissociation, higher charge transfer, and balanced carrier mobility in the blend films, ultimately achieving better PCEs. This work indicates that chlorination of the benzyl group on the terminals can improve the device's performance, implying good application potential in indoor photovoltaics.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 1","pages":"Article 110233"},"PeriodicalIF":9.4,"publicationDate":"2024-07-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141690509","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":"Regulating local electron transfer environment of covalent triazine frameworks through F, N co-modification towards optimized oxygen reduction reaction","authors":"Quanyou Guo , Yue Yang , Tingting Hu, Hongqi Chu, Lijun Liao, Xuepeng Wang, Zhenzi Li, Liping Guo, Wei Zhou","doi":"10.1016/j.cclet.2024.110235","DOIUrl":"10.1016/j.cclet.2024.110235","url":null,"abstract":"<div><div>The high conductivity of electrocatalyst can eliminate the Schottky energy barrier at the interface of heterogeneous phases during an electrocatalytic reaction and accelerate the rapid electron transfer to the catalytic active center. Therefore, the electronic conductivity is a vital parameter for oxygen reduction reaction (ORR). Covalent triazine frameworks (CTFs) have shown great potential application as electrocatalysts in ORR with a merit of the diverse building blocks. However, the intrinsic low conductivity and high impedance of CTFs could be significant setbacks in electrocatalytic application. Herein, CTFs were constructed by introducing F and N co-modification for efficient 2e<sup>−</sup> ORR. Compared with the pristine CTF, the co-presence of F, N could increase the conductivity obviously by 1000-fold. As a result, F-N-CTF exhibits enhanced catalytic performance of H<sub>2</sub>O<sub>2</sub> generation and selectivity towards reaction pathways. This work reveals the importance of conductivity optimization for CTFs and provides guidance for designing high conductivity non-metallic organic semiconductor catalysts for 2e<sup>−</sup> ORR.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 1","pages":"Article 110235"},"PeriodicalIF":9.4,"publicationDate":"2024-07-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141704961","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}
Yuehai Zhi , Chen Gu , Huachao Ji , Kang Chen , Wenqi Gao , Jianmei Chen , Dafeng Yan
{"title":"The advanced development of innovative photocatalytic coupling strategies for hydrogen production","authors":"Yuehai Zhi , Chen Gu , Huachao Ji , Kang Chen , Wenqi Gao , Jianmei Chen , Dafeng Yan","doi":"10.1016/j.cclet.2024.110234","DOIUrl":"10.1016/j.cclet.2024.110234","url":null,"abstract":"<div><div>Photocatalytic technology harnesses solar energy to facilitate chemical transformations, presenting significant potential in energy generation and environmental remediation. However, the conventional O<sub>2</sub> evolution process is hindered by high reaction barriers and inefficiencies, which limit its widespread application. Therefore, exploring novel photocatalytic coupling strategies to replace water oxidation has become a key route to enhance the efficiency of H<sub>2</sub> production. In this review, organic pollutants removal and the valorization of organics as substitutes for water oxidation coupling strategies for photocatalytic H<sub>2</sub> production are comprehensively summarized. These strategies not only circumvent the high reaction barriers associated with O<sub>2</sub> evolution to enhance the H<sub>2</sub> production but also aid in the removing of organic pollutants or synthesis of value-added chemicals. We also present future research directions and underscore the significance of advanced catalyst design, in-depth analysis of reaction mechanisms, and systematic optimization strategies in realizing an efficient and sustainable photocatalytic process. This guidance is anticipated to provide theoretical and practical new insights for the future development of photocatalytic coupling reactions, fostering further explorations in the realm of renewable energy and environmental governance.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 1","pages":"Article 110234"},"PeriodicalIF":9.4,"publicationDate":"2024-07-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141705307","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":"Linear polyurethanes with excellent comprehensive properties from poly(ethylene carbonate) diol","authors":"Xinyu Liu, Jialin Yang, Zonglin He, Jiaoyan Ai, Lina Song, Baohua Liu","doi":"10.1016/j.cclet.2024.110236","DOIUrl":"10.1016/j.cclet.2024.110236","url":null,"abstract":"<div><div>The synthesis of polyurethanes (PUs) from the reaction of low molecular weight poly(ethylene carbonate) diol (PECD) is rarely investigated. This work reports a novel PU with excellent mechanical properties from the solution polymerization of 4,4′-diphenylmethane diisocyanate (MDI) with PECD that was derived from the copolymerization of carbon dioxide (CO<sub>2</sub>) and ethylene oxide (EO). The tensile strength, the elongation at break and 300 % constant tensile strength of the PECD-PU were up to 66 ± 2 MPa, 880 % ± 50 % and 13 MPa, respectively, higher than the control PUs from the reaction of MDI with commercial polyethers or polyesters. The PECD-PU with high CO<sub>2</sub> carbonate content exhibited good solvent resistance and chemical stability. Of importance, the mechanical properties and chemical resistance of PECD-PU were significantly enhanced with the increasing content of CO<sub>2</sub>, <em>i.e.</em>, the carbonate unit in PECD. This work provides comprehensive properties of PECD-derived PUs, indicating that PECD is a competitive precursor for the preparation of PU and has broad application prospects.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 1","pages":"Article 110236"},"PeriodicalIF":9.4,"publicationDate":"2024-07-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141695606","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}
Jinqiang Gao , Haifeng Yuan , Xinjuan Du , Feng Dong , Yu Zhou , Shengnan Na , Yanpeng Chen , Mingyu Hu , Mei Hong , Shihe Yang
{"title":"Methanol steam mediated corrosion engineering towards high-entropy NiFe layered double hydroxide for ultra-stable oxygen evolution","authors":"Jinqiang Gao , Haifeng Yuan , Xinjuan Du , Feng Dong , Yu Zhou , Shengnan Na , Yanpeng Chen , Mingyu Hu , Mei Hong , Shihe Yang","doi":"10.1016/j.cclet.2024.110232","DOIUrl":"10.1016/j.cclet.2024.110232","url":null,"abstract":"<div><div>Rational design of viable routes to obtain efficient and stable oxygen evolution reaction (OER) electrocatalysts remains challenging, especially under industrial conditions. Here, we provide a solvent-steam assisted corrosion engineering strategy to directly fabricate high-entropy NiFe-LDH with spatially resolved structural order. Ammonium fluoride in methanol steam enables the formation of nanosheets while Fe<sup>3+</sup> effectively enhances their adhesion to the semi-sacrificial nickel-iron foam (NFF), thereby conjuring up a NiFe-LDH@NFF catalyst that exhibits remarkable adaptability to robust electrochemical activation yet with excellent stability. Comprehensive measurements reveal the <em>in-situ</em> formation of high-valance metal oxyhydroxide and the enhancement of adsorption-desorption process. Under the industrial condition (6 mol/L KOH, 60 °C), the NiFe-LDH@NFF exhibits excellent activity of 50 mA/cm<sup>2</sup> at 1.55 V and high durability of over 120 h at 200 mA/cm<sup>2</sup>. We anticipate that the steam assisted strategy could promote the development of efficient non-precious electrocatalysts for hydrogen energy.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 1","pages":"Article 110232"},"PeriodicalIF":9.4,"publicationDate":"2024-07-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141715263","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}
Makhloufi Zoulikha , Zhongjian Chen , Jun Wu , Wei He
{"title":"Approved delivery strategies for biopharmaceuticals","authors":"Makhloufi Zoulikha , Zhongjian Chen , Jun Wu , Wei He","doi":"10.1016/j.cclet.2024.110225","DOIUrl":"10.1016/j.cclet.2024.110225","url":null,"abstract":"<div><div>In recent years, biopharmaceuticals have witnessed remarkable advancements, transforming the landscape of therapeutic interventions. Biopharmaceuticals encompassing therapeutics generated through cutting-edge biotechnological methods have shown promising therapeutic outcomes. However, their clinical success hinges significantly on overcoming drug delivery challenges related to stability, intracellular delivery, immunogenicity, and pharmacokinetic properties. Herein, we provide an overview of various marketed macromolecules, including nucleic acids, and immunotherapeutic agents such as cytokines and monoclonal antibodies, as well as other therapeutic peptides/proteins like enzymes, hormones, and coagulation factors. Our primary focus is on elucidating the delivery challenges associated with these macromolecules and highlighting the pivotal role played by drug delivery platforms in the development of currently marketed products, offering valuable insights for both scientific research and the pharmaceutical industry.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 2","pages":"Article 110225"},"PeriodicalIF":9.4,"publicationDate":"2024-07-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141695194","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}
Lili Zhang , Hui Gao , Gong Zhang , Yuning Dong , Kai Huang , Zifan Pang , Tuo Wang , Chunlei Pei , Peng Zhang , Jinlong Gong
{"title":"Cross-section design of the flow channels in membrane electrode assembly electrolyzer for CO2 reduction reaction through numerical simulations","authors":"Lili Zhang , Hui Gao , Gong Zhang , Yuning Dong , Kai Huang , Zifan Pang , Tuo Wang , Chunlei Pei , Peng Zhang , Jinlong Gong","doi":"10.1016/j.cclet.2024.110204","DOIUrl":"10.1016/j.cclet.2024.110204","url":null,"abstract":"<div><div>Membrane electrode assembly (MEA) is widely considered to be the most promising type of electrolyzer for the practical application of electrochemical CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR). In MEAs, a square-shaped cross-section in the flow channel is normally adopted, the configuration optimization of which could potentially enhance the performance of the electrolyzer. This paper describes the numerical simulation study on the impact of the flow-channel cross-section shapes in the MEA electrolyzer for CO<sub>2</sub>RR. The results show that wide flow channels with low heights are beneficial to the CO<sub>2</sub>RR by providing a uniform flow field of CO<sub>2</sub>, especially at high current densities. Moreover, the larger the electrolytic cell, the more significant the effect is. This study provides a theoretical basis for the design of high-performance MEA electrolyzers for CO<sub>2</sub>RR.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 1","pages":"Article 110204"},"PeriodicalIF":9.4,"publicationDate":"2024-07-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141703617","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}
Binhan Zhao , Zheng Li , Lan Zheng , Zhichao Ye , Yuyang Yuan , Shanshan Zhang , Bo Liang , Tianyu Li
{"title":"Recent progress in the biomedical application of PEDOT:PSS hydrogels","authors":"Binhan Zhao , Zheng Li , Lan Zheng , Zhichao Ye , Yuyang Yuan , Shanshan Zhang , Bo Liang , Tianyu Li","doi":"10.1016/j.cclet.2024.109810","DOIUrl":"https://doi.org/10.1016/j.cclet.2024.109810","url":null,"abstract":"<div><p>Bioelectronics have gained substantial research attention owing to their potential applications in health monitoring and diagnose, and greatly promoted the development of biomedicine. Recently, poly(3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS) hydrogels have arose as a promising candidate for the next-generation bioelectronic interface due to its high-conductivity, versatility, flexibility and biocompatibility. In this review, we highlight the recent advances of PEDOT:PSS hydrogels, including the gelation methods and modification strategies, and summarize their wide applications in different type of sensors and tissue engineering in detail. We expect that this work will provide valuable information regarding the functionalizations and applications of PEDOT:PSS hydrogels.</p></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"35 10","pages":"Article 109810"},"PeriodicalIF":9.4,"publicationDate":"2024-07-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141583161","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}