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A TEMPO-N3 Complex Enables the Electrochemical C-H Azidation of N-Heterocycles through the Cleavage of Alkoxyamines. 一种 TEMPO-N3 复合物可通过烷氧基胺的裂解实现 N-杂环的电化学 C-H Azidation。
IF 7.5 2区 化学
ChemSusChem Pub Date : 2024-11-22 DOI: 10.1002/cssc.202402139
Sumit Biswas, Subhadeep Ghosh, Indrajit Das
{"title":"A TEMPO-N<sub>3</sub> Complex Enables the Electrochemical C-H Azidation of N-Heterocycles through the Cleavage of Alkoxyamines.","authors":"Sumit Biswas, Subhadeep Ghosh, Indrajit Das","doi":"10.1002/cssc.202402139","DOIUrl":"10.1002/cssc.202402139","url":null,"abstract":"<p><p>A TEMPO-N<sub>3</sub> charge-transfer complex enables the electrochemical C-H azidation of various N-heterocycles. The TEMPO<sup>+</sup> ion, generated from TEMPO, assists in producing N<sub>3</sub> <sup>⋅</sup> by forming a TEMPO-N<sub>3</sub> complex with N<sub>3</sub> <sup>-</sup>. The formation of this complex is supported by UV-vis absorption spectra, cyclic voltammetry studies, and ESI-HRMS studies. The reaction likely proceeds by forming a highly labile azidooxygenation adduct, which undergoes oxidative alkoxyamine mesolytic cleavage. Subsequent deprotonation of the resulting carbocation exclusively produces the azidation product. It is important to note that substituted olefins generally yield azidooxygenation or diazidation as the final product. Our study demonstrates that N-heterocycles deliver a selective monoazidation product, possibly due to steric reasons. ESI-HRMS studies provide evidence for forming azidooxygenation and alkoxyamine radical cation adducts. The regio- and chemoselectivity of this azidation reaction using the TEMPO-N<sub>3</sub> complex have been discussed.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402139"},"PeriodicalIF":7.5,"publicationDate":"2024-11-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142685573","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Polyethyleneimine-Templated ZIF-8 Nanoparticles Impart the Nanofiltration Membrane with High Mg2+/Li+ Separation Performance. PEI-emplated ZIF-8 纳米粒子赋予 NF 膜很高的 Mg2+/Li+ 分离性能。
IF 7.5 2区 化学
ChemSusChem Pub Date : 2024-11-22 DOI: 10.1002/cssc.202402264
Yanan Dong, Ju Bai, Luqi Xiao, Shangqing Chen, Lu Bai, Huaigang Cheng, Linglong Shan, Junfeng Wang, Yi Nie
{"title":"Polyethyleneimine-Templated ZIF-8 Nanoparticles Impart the Nanofiltration Membrane with High Mg<sup>2+</sup>/Li<sup>+</sup> Separation Performance.","authors":"Yanan Dong, Ju Bai, Luqi Xiao, Shangqing Chen, Lu Bai, Huaigang Cheng, Linglong Shan, Junfeng Wang, Yi Nie","doi":"10.1002/cssc.202402264","DOIUrl":"10.1002/cssc.202402264","url":null,"abstract":"<p><p>MOFs-modified nanofiltration (NF) membranes have been gained a lot of attention due to their favorable permeability and ion separation performance. Nevertheless, the prevailing preparation techniques are afflicted by the incompatibility of MOFs with polymers and the facile loss of MOFs. In this work, polyethyleneimine (PEI)-templated ZIF-8 (PEI-ZIF-8) was synthesized and incorporated into the PEI aqueous solution, then interfacial polymerized with trimesoyl chloride (TMC) to obtain the PEI-ZIF-8 modified polyamide NF membrane. This PEI modified strategy could endow the ZIF-8 nanoparticles with positively charged properties to avoid the aggregation and increase the interfacial compatibility with the polyamide. Meanwhile, the appropriate pore size of ZIF-8 (3.4 Å), which is between the hydration sheath surrounding of Li<sup>+</sup> (2 Å) and Mg<sup>2+</sup> (4.2 Å) impart the membrane with precise Mg<sup>2+</sup>/Li<sup>+</sup> separation ability. The optimal PEI-ZIF-8-TMC membrane exhibits a permeance of 9 L/h m<sup>2</sup>bar and a Mg<sup>2+</sup>/Li<sup>+</sup> separation factor (SF) of 19, both of which surpass the performance of the pure PEI-TMC membrane, which has a permeance of 4 L/h m<sup>2</sup>bar and a Mg<sup>2+</sup>/Li<sup>+</sup> separation factor of 11. Meanwhile, the membrane exhibited excellent long-term stability of 85 h. This novel approach to preparing MOFs-modified NF membrane represents a promising avenue for the separation of lithium and magnesium.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402264"},"PeriodicalIF":7.5,"publicationDate":"2024-11-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142685575","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Polymer Networks Assembled by Ruthenium Catalysts for Enhanced Water Splitting Performance in Calixarene Dye-Sensitized Photoelectrochemical Cells. 钌催化剂组装的聚合物网络用于增强钙钛矿染料敏化光电化学电池的水分离性能。
IF 7.5 2区 化学
ChemSusChem Pub Date : 2024-11-21 DOI: 10.1002/cssc.202402395
Xiao-Lin Wang, Li-Lin Tan, Yang Liu, Jia-Xin Liu, Xin-Ao Li, Zi-Zhan Liang, Jian-Feng Huang, Jun-Min Liu
{"title":"Polymer Networks Assembled by Ruthenium Catalysts for Enhanced Water Splitting Performance in Calixarene Dye-Sensitized Photoelectrochemical Cells.","authors":"Xiao-Lin Wang, Li-Lin Tan, Yang Liu, Jia-Xin Liu, Xin-Ao Li, Zi-Zhan Liang, Jian-Feng Huang, Jun-Min Liu","doi":"10.1002/cssc.202402395","DOIUrl":"10.1002/cssc.202402395","url":null,"abstract":"<p><p>Metal-free photosensitizers for the construction of low-cost and eco-friendly dye-sensitized photoelectrochemical cells (DSPECs) have recently been greatly improved, but the optimization of water oxidation catalysts (WOCs) used in DSPECs based on metal-free dyes has received little attention. Herein, a series of polymer networks (RuTPA, RuCz, RuPr and RuTz) assembled by ruthenium WOCs (RuCHO) with various organic donors are constructed and combined with calixarene dyes to prepare DSPEC devices. The FTO|TiO<sub>2</sub>|C4BTP+RuTPA photoanode shows the best performance with 85 % Faraday efficiency for oxygen production and 477 μA cm<sup>-2</sup> photocurrent density after 200 s chopping irradiation at 0 V vs. Ag/AgCl, one of the highest records among other reported dye-sensitized photoanodes. Compared to monomeric RuCHO, Ru-based polymers with lower Ru content have higher activity and stability due to their rapid electron transfer and anti-aggregation ability. Meanwhile, RuTPA loaded electrodes show better performance due to the lower overpotential of the water oxidation reaction caused by the higher electron donating ability of its donor. This pioneering work incorporates Ru polymer networks as WOCs into the calixarene-sensitized DSPEC system, which has significant potential as a highly efficient and stable photoelectrochemical water splitting device.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402395"},"PeriodicalIF":7.5,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142680397","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Efficient Alkaline Freshwater/Seawater Hydrogen Production via Heterogeneous N-Doped FeMoO4/Mo2N Rod-Shaped Electrocatalysts. 通过异质 N 掺杂 FeMoO4/Mo2N 棒状电催化剂高效生产碱性淡水/海水氢气。
IF 7.5 2区 化学
ChemSusChem Pub Date : 2024-11-21 DOI: 10.1002/cssc.202401425
Yanxiang He, Meilian Tu, Weijiang Gan, Zhixiao Zhu, Muhammad Mushtaq, Mohammad Al-Mamun, Jianqiu Deng, Hao Yang, Zhongmin Wang, M-Sadeeq Balogun
{"title":"Efficient Alkaline Freshwater/Seawater Hydrogen Production via Heterogeneous N-Doped FeMoO<sub>4</sub>/Mo<sub>2</sub>N Rod-Shaped Electrocatalysts.","authors":"Yanxiang He, Meilian Tu, Weijiang Gan, Zhixiao Zhu, Muhammad Mushtaq, Mohammad Al-Mamun, Jianqiu Deng, Hao Yang, Zhongmin Wang, M-Sadeeq Balogun","doi":"10.1002/cssc.202401425","DOIUrl":"https://doi.org/10.1002/cssc.202401425","url":null,"abstract":"<p><p>Durable and efficient Fe-based electrocatalysts in alkaline freshwater/seawater electrolysis is highly desirable but persists a significant challenge. Herein, we report a durable and robust heterogenous nitrogen-doped FeMoO<sub>4</sub>/Mo<sub>2</sub>N rod-shaped catalyst on nickel foam (denoted NF@FMO/MN) affording hydrogen evolution reaction (HER) low overpotentials of 23/29 mV@10 mA cm<sup>-2</sup> and 112/159 mV@100 mA cm<sup>-2</sup> in both alkaline freshwater/seawater electrolytes, respectively. These results are significantly superior to the pristine FeMoO<sub>4</sub> catalyst. Theoretical calculations consistently reveals that the combination of N-FeMoO<sub>4</sub> and Mo<sub>2</sub>N effectively reduces water activation energy barrier, modulates the sluggish water-dissociation kinetics and accelerates the hydrogen adsorption process for efficient HER. The enhanced HER performance of the as-designed NF@FMO/MN catalyst is attributed to the in situ hetero-interfacial engineering between N-doped FeMoO<sub>4</sub> and Mo<sub>2</sub>N. This present work nurtures the progress of FeMo-based electrocatalysts in alkaline freshwater/seawater electrolysis.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401425"},"PeriodicalIF":7.5,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142685574","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Metal-free N, P-Codoped Carbon for Syngas Production with Tunable Composition via CO2 Electrolysis: Addressing the Competition Between CO2 Reduction and H2 Evolution. 无金属 N、P-掺杂碳通过二氧化碳电解生产成分可调的合成气:解决二氧化碳还原和 H2 喷射之间的竞争问题。
IF 7.5 2区 化学
ChemSusChem Pub Date : 2024-11-21 DOI: 10.1002/cssc.202402249
Ryuji Takada, Hiroyuki Okada, Kotaro Narimatsu, Koji Miyake, Yoshiaki Uchida, Etsushi Tsuji, Norikazu Nishiyama
{"title":"Metal-free N, P-Codoped Carbon for Syngas Production with Tunable Composition via CO2 Electrolysis: Addressing the Competition Between CO2 Reduction and H2 Evolution.","authors":"Ryuji Takada, Hiroyuki Okada, Kotaro Narimatsu, Koji Miyake, Yoshiaki Uchida, Etsushi Tsuji, Norikazu Nishiyama","doi":"10.1002/cssc.202402249","DOIUrl":"https://doi.org/10.1002/cssc.202402249","url":null,"abstract":"<p><p>Electroreduction of carbon dioxide into value-added fine chemicals is a promising technique to realize the carbon cycle. Recently, metal-free heteroatom doped carbons are proposed as promising cost-effective electrocatalysts for CO2 reduction reaction (CO2RR). However, the lack of understanding of the active site prevents the realization of a high-performance electrocatalyst for the CO2RR. Herein, we synthesized metal-free N, P co-doped carbons (NPCs) for producing syngas, which is composed of H2 and CO, by CO2 electrolysis using inexpensive bio-based raw materials via simple pyrolysis. The syngas ratio (H2/CO) can be controlled within the high demand range (0.3-4) at low potentials using NPCs by tuning the N and P contents. In comparison with only N doping or P doping, N and P co-doping has a positive impact on improving CO2RR activity. Experimental analysis and density functional theoretical (DFT) calculations revealed that negatively charged C atoms adjacent to N and P atoms are the most favorable active sites for CO2-to-CO conversion compared to pyridinic N on N, P co-doped carbon. Introducing N atoms generates the preferable CO2 adsorption site, and P atoms contribute to decreasing the Gibbs free energy barrier for key *COOH intermediates adsorbed on the negatively charged C atoms.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402249"},"PeriodicalIF":7.5,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142680376","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Green Electrochemical Point-of-Care Devices: Transient Materials and Sustainable Fabrication Methods. 绿色电化学护理点设备:瞬态材料和可持续制造方法。
IF 7.5 2区 化学
ChemSusChem Pub Date : 2024-11-21 DOI: 10.1002/cssc.202401101
David Batet, Gemma Gabriel
{"title":"Green Electrochemical Point-of-Care Devices: Transient Materials and Sustainable Fabrication Methods.","authors":"David Batet, Gemma Gabriel","doi":"10.1002/cssc.202401101","DOIUrl":"10.1002/cssc.202401101","url":null,"abstract":"<p><p>The spread of point-of-care (PoC) diagnostic tests using electrochemical sensors poses a significant environmental challenge, especially in limited-resource settings due to the lack of waste management infrastructure. This issue is expected to intensify with the emergence of the Internet of Medical Things (IoMT), necessitating eco-friendly solutions for disposable devices. This review discusses efforts to develop green and sustainable PoC diagnostic devices, clarifying terms like biodegradability and transient electronics. It explores potential transient and biodegradable materials and fabrication technologies, emphasizing sustainable electronics with low-energy consumption and low-carbon footprint techniques, particularly favoring printing methods. The review highlights examples of necessary electronic components containing biodegradable materials for electrochemical PoC devices and discusses their role in device sustainability. Finally, it examines the feasibility of integrating these components and technologies into comprehensive biodegradable PoC devices, addressing the imminent need for eco-friendly solutions in diagnostic testing. This comprehensive discussion serves as a guide for researchers and developers striving to mitigate the environmental impact of PoC testing in the era of IoMT and personalized medicine.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401101"},"PeriodicalIF":7.5,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142680237","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Cascade Catalytic Systems for Converting CO2 into C2+ Products. 将二氧化碳转化为 C2+ 产品的级联催化系统。
IF 7.5 2区 化学
ChemSusChem Pub Date : 2024-11-20 DOI: 10.1002/cssc.202401916
Qiaochu Shi, Boyu Zhang, Zhenhua Wu, Dong Yang, Hong Wu, Jiafu Shi, Zhongyi Jiang
{"title":"Cascade Catalytic Systems for Converting CO<sub>2</sub> into C<sub>2+</sub> Products.","authors":"Qiaochu Shi, Boyu Zhang, Zhenhua Wu, Dong Yang, Hong Wu, Jiafu Shi, Zhongyi Jiang","doi":"10.1002/cssc.202401916","DOIUrl":"10.1002/cssc.202401916","url":null,"abstract":"<p><p>The excessive emission and continuous accumulation of CO<sub>2</sub> have precipitated serious social and environmental issues. However, CO<sub>2</sub> can also serve as an abundant, inexpensive, and non-toxic renewable C<sub>1</sub> carbon source for synthetic reactions. To achieve carbon neutrality and recycling, it is crucial to convert CO<sub>2</sub> into value-added products through chemical pathways. Multi-carbon (C<sub>2+</sub>) products, compared to C<sub>1</sub> products, offer a broader range of applications and higher economic returns. Despite this, converting CO<sub>2</sub> into C<sub>2+</sub> products is difficult due to its stability and the high energy required for C-C coupling. Cascade catalytic reactions offer a solution by coordinating active components, promoting intermediate transfers, and facilitating further transformations. This method lowers energy consumption. Recent advancements in cascade catalytic systems have allowed for significant progress in synthesizing C<sub>2+</sub> products from CO<sub>2</sub>. This review highlights the features and advantages of cascade catalysis strategies, explores the synergistic effects among active sites, and examines the mechanisms within these systems. It also outlines future prospects for CO<sub>2</sub> cascade catalytic synthesis, offering a framework for efficient CO<sub>2</sub> utilization and the development of next-generation catalytic systems.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401916"},"PeriodicalIF":7.5,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142674662","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
A Solid Electrolyte Based on Sodium-Doped Li4-xNaxTi5O12 with PVDF for Solid State Lithium Metal Battery. 基于钠掺杂 Li4-xNaxTi5O12 与 PVDF 的固态电解质,用于固态锂金属电池。
IF 7.5 2区 化学
ChemSusChem Pub Date : 2024-11-20 DOI: 10.1002/cssc.202401755
Qiyue Chen, Haitao Lv, Jun Peng, Qi Zhou, Wenzhuo Wu, Jing Wang, Lili Liu, Lijun Fu, Yuhui Chen, Yuping Wu
{"title":"A Solid Electrolyte Based on Sodium-Doped Li<sub>4-x</sub>Na<sub>x</sub>Ti<sub>5</sub>O<sub>12</sub> with PVDF for Solid State Lithium Metal Battery.","authors":"Qiyue Chen, Haitao Lv, Jun Peng, Qi Zhou, Wenzhuo Wu, Jing Wang, Lili Liu, Lijun Fu, Yuhui Chen, Yuping Wu","doi":"10.1002/cssc.202401755","DOIUrl":"10.1002/cssc.202401755","url":null,"abstract":"<p><p>Solid-state batteries (SSBs) present a potential pathway for advancing next-generation lithium batteries, characterized by exceptional energy density and enhanced safety performance. Solid-state electrolytes have been extensively researched, yet an affordable option with outstanding electrochemical performance is still lacking. In this work, Li<sub>4-x</sub>Na<sub>x</sub>Ti<sub>5</sub>O<sub>12</sub> (LNTO)-based composite solid electrolytes (CSEs) were developed to enhance the interface stability and electronic insulation. The CSE is composed of Li<sub>3.88</sub>Na<sub>0.12</sub>Ti<sub>5</sub>O<sub>12</sub> (LNTO3) and poly (vinylidene fluoride) (PVDF) with a proportion of 20 wt % exhibited high ionic conductivity (4.49×10<sup>-4</sup> S cm<sup>-1</sup> at a temperature value equal to 35 °C), high ionic transfer number (equal to 0.72), low activation energy (equal to 0.192 eV), and favorable compatibility with the Li metal anode. The Li|LNTO3|LiFePO<sub>4</sub> cell, tested at a 0.5 C current density, demonstrated 154.5 mAh g<sup>-1</sup> of outstanding cycling stability for 200 cycles, capacity retention of 97.6 % along with a Coulombic efficiency of over 99 %, as well as a significant average specific capacity of 127.8 mAh g<sup>-1</sup> over 400 cycles at 5 C. The Li|LNTO3|LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> (NCM811) cell could also operate over 100 cycles at 1 C. This study offers an effective method for preparing commercial CSEs for SSBs.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401755"},"PeriodicalIF":7.5,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142674660","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Engineering Delocalized Polarizations in Metal Oxide Electrodes with Conducting Polymers for Efficient and Durable Water-Splitting. 利用导电聚合物在金属氧化物电极中实现局部极化,从而实现高效持久的分水。
IF 7.5 2区 化学
ChemSusChem Pub Date : 2024-11-20 DOI: 10.1002/cssc.202401881
Hyunji Oh, Ji-Woo Park, Jiyeoung Choi, Young-Wan Ju, Changmin Kim, Jeeyoung Shin
{"title":"Engineering Delocalized Polarizations in Metal Oxide Electrodes with Conducting Polymers for Efficient and Durable Water-Splitting.","authors":"Hyunji Oh, Ji-Woo Park, Jiyeoung Choi, Young-Wan Ju, Changmin Kim, Jeeyoung Shin","doi":"10.1002/cssc.202401881","DOIUrl":"10.1002/cssc.202401881","url":null,"abstract":"<p><p>Oxygen evolution reaction is a pivotal anodic reaction for electrolysis, however, it remains the obstacle from its sluggish reaction kinetics originating from multiple electron transfer pathways at electrochemical interfaces. Especially, it remains a challenge to achieve stable operation at elevated current densities as electrodes suffer oxidative environment in corrosive conditions. Herein, we report that the conducting polymer polypyrrole electrodeposited Pr<sub>0.7</sub>Sr<sub>0.3</sub>CoO<sub>3</sub> perovskite oxides for durable oxygen evolution electrodes. We found that the conducting polymer electrodeposited oxides exhibited a highly durable electrochemical oxygen evolution performance maintaining >99 % of initial activities during the accelerated durability test. Meanwhile, bare metal oxides presented significant performance drops (<6 % of initial activities) over the consecutive 20,000 accelerated durability test. High-resolution transmission electron microscope images identified the maintenance of high crystallinity of the heterostructure, suggesting that the electrodeposited pPy clusters can effectively delocalize highly polarized electrodes preventing material corrosion. The overall water electrolysis experiments further demonstrated that the heterostructure showed excellent stability at the high current density of 100 mA cm<sup>-2</sup> over 700 hours. This marks the first report of the delocalized polarization benefiting from conducting polymers for durable oxygen evolution for perovskite oxides, suggesting great potential for scalable water electrolysis.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401881"},"PeriodicalIF":7.5,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142680236","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Exploiting Acetal Moieties for the Synthesis of Degradable-On-Demand Polymeric Architectures. 利用乙缩醛分子合成可按需降解的聚合物结构。
IF 7.5 2区 化学
ChemSusChem Pub Date : 2024-11-20 DOI: 10.1002/cssc.202402154
Angela Romano, Stefano Frattini, Roberto Miani, Claudio Gioia, Annamaria Celli, Laura Sisti
{"title":"Exploiting Acetal Moieties for the Synthesis of Degradable-On-Demand Polymeric Architectures.","authors":"Angela Romano, Stefano Frattini, Roberto Miani, Claudio Gioia, Annamaria Celli, Laura Sisti","doi":"10.1002/cssc.202402154","DOIUrl":"10.1002/cssc.202402154","url":null,"abstract":"<p><p>Developing polymers with labile bonds has attracted increasing attention since it can favor the chemical recycling into oligomers or even the starting monomers that could be recovered and re-used. Different chemical bonds can break upon exposure to external stimuli, such as thermal, UV, or chemical triggers. Among these, the acetal bond can degrade under mild acidic conditions. This study focuses on the synthesis of polymers constituted by acetal moieties suitable for triggered depolymerization. In particular, the solvent-less polyaddition of 1,4-butanediol and 1,4-butanediol divinyl ether was developed and optimized using a heterogeneous catalyst (Amberlyst 15) at 100 °C. The best reaction conditions in terms of catalyst loading and reagent ratio were determined through a Design-of-Experiment aiming to achieve high conversion, low polydispersity, and desirable molecular weight. The resulting material presented an amorphous character and thermal stability up to 220 °C. It was confirmed responsive in an acidic environment, being completely hydrolyzed in 42 days, while remaining stable at neutral and basic pH. The obtained results represent a proof of concept for the design of pH-responsive materials through solventless, and scalable processes. The acetal moiety may be further exploited to achieve architectures presenting a sustainable end-of-life by implementing a recycling-by-design approach for new adhesives or novel degradable thermosetting materials.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402154"},"PeriodicalIF":7.5,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142674664","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","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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