{"title":"Recovering noble metals from waste streams using porous organic frameworks for heterogeneous catalysis","authors":"Yu Pan, Michelle Åhlén, Maria Strømme, Chao Xu","doi":"10.1007/s11426-024-2021-5","DOIUrl":"10.1007/s11426-024-2021-5","url":null,"abstract":"<div><p>Recovering noble metals from waste resources and incorporating them into catalysts stands out as a promising strategy for advancing sustainability within the catalysis field. This review provides a comprehensive overview of recent investigations into noble metal recovery from waste streams, specifically employing porous organic frameworks (POFs). Additionally, the study delves into the utilization of the resultant composites, enriched with noble metals, in heterogeneous catalysis. Moreover, we offer insights into the challenges faced and outline prospects for the practical implementation of extracting noble metal catalysts from waste streams using POFs, aiming to develop cost-effective, sustainable, and efficient heterogeneous catalysts.\u0000</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"67 11","pages":"3578 - 3587"},"PeriodicalIF":10.4,"publicationDate":"2024-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://link.springer.com/content/pdf/10.1007/s11426-024-2021-5.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142519070","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Electrochemical impedance spectroscopy analysis to accelerate electrocatalytic system innovation","authors":"Hanbing Zhu, Yinghuan Liu, Wenxin Guo, Jinyu Zheng, Yao Zheng, Serhiy Cherevko, Cheng Tang, Qiang Zhang","doi":"10.1007/s11426-024-2314-9","DOIUrl":"10.1007/s11426-024-2314-9","url":null,"abstract":"<div><p>Electrochemical impedance spectroscopy (EIS) is a well-established non-destructive characterization technique for assessing the efficacy of electrochemical energy storage and conversion systems. Electrocatalytic systems based on proton exchange membrane (PEM), including PEM fuel cells and PEM water electrolyzers, play a crucial role in renewable energy conversion through electricity–hydrogen interconversion. EIS, along with its derived analysis methods—equivalent circuit model (ECM), distribution of relaxation time (DRT), and dynamic EIS (DEIS), is widely utilized to extract valuable kinetics and impedance data. The acquired information affords critical insights into processes such as mass transfer, charge transfer, and proton transfer within PEM systems. This mini review surveys the role of EIS in optimizing components and investigating operational conditions to enhance the efficiency of PEM systems. In addition, it encapsulates the principles and applications of EIS-based methods like DRT and DEIS, highlighting their potential in the practical application of PEM systems.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"67 12","pages":"3964 - 3975"},"PeriodicalIF":10.4,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142757975","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":"Nucleophilic trifluoromethylation with CF3H/LiHMDS: probing the nucleophilic reactivity of LiCF3 species","authors":"Yangfan Liu, Xiu Wang, Chuanfa Ni, Jinbo Hu","doi":"10.1007/s11426-024-2289-7","DOIUrl":"10.1007/s11426-024-2289-7","url":null,"abstract":"<div><p>The nucleophilic trifluoromethylation involving trifluoromethyllithium (LiCF<sub>3</sub>) species has been an open question since Haszeldine attempted to prepare LiCF<sub>3</sub> in 1949. Indeed, LiCF<sub>3</sub> has been used for electrophilic difluoromethylene transfer processes (<i>via</i> elimination of fluoride ions) since 2010. Herein, we demonstrated that by using a polar solvent such as dimethylformamide (DMF) or hexamethylphosphoramide (HMPA) as the lithium chelator, the <i>in situ</i> deprotonation of fluoroform (HCF<sub>3</sub>) with lithium hexamethyldisilazide (LiHMDS) could generate a tamed LiCF<sub>3</sub> species that is sufficiently persistent to undergo nucleophilic trifluoromethylation reaction. The nucleophilic reactivity of LiCF<sub>3</sub> species was probed with several electrophiles, including arylsulfonyl fluorides, diaryl ketones, and silyl chlorides. The synthetic utility of this method is demonstrated with the efficient synthesis of highly valuable triflones that are otherwise difficult to synthesize from HCF<sub>3</sub> using potassium or sodium bases. This work not only showcases a new protocol for the utilization of fluoroform (an industrial waste with high global warming potential) as the trifluoromethylation reagent, but also provides intriguing insights into the harnessing of nucleophilic reactivity of the transient LiCF<sub>3</sub> species.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 2","pages":"505 - 512"},"PeriodicalIF":10.4,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://link.springer.com/content/pdf/10.1007/s11426-024-2289-7.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142249199","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Visible-light-induced organocatalyzed C(sp2)-H bond functionalization of 1,3-azoles with trifluoroacetylsilanes","authors":"Zhengyu Li, Zeguo Zhang, Zhihan Zhang, Gang Zhou, Yizhi Zhang, Shanshan Liu, Xiao Shen","doi":"10.1007/s11426-024-2203-5","DOIUrl":"10.1007/s11426-024-2203-5","url":null,"abstract":"<div><p>Previous carbene insertion to C-H bonds of 1,3-azoles relied on metal carbene species. Herein, we report a metal-free C(sp<sup>2</sup>)-H bond functionalization of 1,3-azoles with trifluoroacetylsilanes. The reaction features mild conditions, broad substrate scope and wide functional group tolerance. The mechanistic study supports that the success of the reaction is probably attributed to the dual roles of trifluoroacetylsilanes under the photocatalyzed conditions: generating carbenes which undergo cyclopropanation and generating biradicals which promote ring-opening aromatization of the <i>in situ</i> generated fused cyclopropanes.\u0000</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"67 11","pages":"3662 - 3668"},"PeriodicalIF":10.4,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142518481","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":"XAFS method for the structural characterization of single atom catalysts","authors":"Houhong Song, Ziyu Song, Wenting Zhou, Siyu Yao","doi":"10.1007/s11426-024-2257-6","DOIUrl":"https://doi.org/10.1007/s11426-024-2257-6","url":null,"abstract":"<p>Single atom catalysts (SACs) have become a hot topic in catalysis research due to their 100% atomic utilization, unique coordination environment, and superior catalytic performance. To explain the special catalytic behavior of SACs and maximize the advantages of single atom configurations, understanding the structure-performance relationship of SACs at the atomic level is key to the research. X-ray absorption fine structure (XAFS) provides an irreplaceable method for characterizing SACs, which can be applied to almost all transition-metal SACs and can obtain rich structural information about atomistic structures and electronic properties. In this review, starting from the basic principles of XAFS technology, we discuss the application of extended X-ray absorption fine structure (EXAFS) and X-ray absorption near edge structure (XANES) spectroscopy in the study of the local coordination, symmetry, hybrid of orbitals, oxidation state, charge transfer and many other structural and electronic properties. After that, we introduce the emerging advanced X-ray spectroscopy methods that improve characterization capabilities and compensate for the shortcomings of traditional XAFS methods in SAC research, and then discuss <i>in-situ</i> and <i>operando</i> experimental techniques for SAC characterization to monitor the dynamic structure of the active sites in the presence of reactants under reaction conditions.</p>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"12 1","pages":""},"PeriodicalIF":9.445,"publicationDate":"2024-09-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142249231","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":"Surface ligand-promoted heterogeneous CO2 catalysis","authors":"Zhe Lu, Lu Wang","doi":"10.1007/s11426-024-2205-y","DOIUrl":"10.1007/s11426-024-2205-y","url":null,"abstract":"<div><p>Heterogeneous CO<sub>2</sub> catalysis towards the synthesis of high-value products provides a potent pathway for achieving carbon neutrality. The distinctive attributes of surface ligands allow for highly effective tuning of the kinetics and mechanisms to enhance CO<sub>2</sub> conversion performance. In this review, the catalytic contributions of surface ligands from the view of structure modulation, mechanism modulation, mass transfer, and energy transfer were summarized. The relationships between surface ligands and the performance of functionalized catalysts were further explored. Subsequently, the applications of hydrocarbon chain spacer, hydroxyl and amino as terminal, and SiO<sub><i>x</i></sub> ligand in thermal, photo, and photothermal CO<sub>2</sub> conversion were investigated. By examining the current limitations and advancements, we concluded with insights into potential future research directions that focus on the development of precisely tuned active sites for highly efficient CO<sub>2</sub> conversion.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 2","pages":"444 - 457"},"PeriodicalIF":10.4,"publicationDate":"2024-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142249233","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}
Sheng Jiang, Shaobing Xiong, Shuaifei Mao, Yefan Zhang, Dongyang Zhao, Xiaomeng You, Vladimir Gaishun, Dmitry Kovalenk, Qinye Bao
{"title":"Light-activated tautomeric transition enhanced buried heterointerface for highly efficient and ultraviolet robust perovskite solar cells","authors":"Sheng Jiang, Shaobing Xiong, Shuaifei Mao, Yefan Zhang, Dongyang Zhao, Xiaomeng You, Vladimir Gaishun, Dmitry Kovalenk, Qinye Bao","doi":"10.1007/s11426-024-2194-0","DOIUrl":"10.1007/s11426-024-2194-0","url":null,"abstract":"<div><p>The buried heterointerface of perovskite solar cells (PSCs) suffers from serious nonradiative recombination and ultraviolet (UV) light stress, relentlessly limiting further increase in their power conversion efficiency and operational stability. Herein, we develop an emerging strategy of incorporating a thin UV-activated tautomeric transition layer onto underlying charge transport layer and then depositing perovskite layer to construct an efficient hole-selective buried heterojunction. It is revealed that the UV-activated tautomeric transition interlayer not only improves upper perovskite crystallinity, diminishes thermionic loss for collecting hole and passivates defect site at such buried contact that significantly promote charge transport and suppress nonradiative recombination, but also effectively protects adjacent perovskite from UV degradation through “UV sunscreen” effect. As a result, we report a remarkably enhanced efficiency of 24.76% compared to 22.02% of the control device. More importantly, the achieved high-efficiency PSC features excellent resistance against UV radiation at 365 nm of 100 and 850 mW cm<sup>−2</sup>, which are approximately 21 and 184 times of UV flux (4.6 mW cm<sup>−2</sup>) under AM 1.5G solar illumination. This work provides a promising approach of strengthening buried heterointerface for simultaneous realization of highly efficient and UV robust PSCs.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 2","pages":"723 - 732"},"PeriodicalIF":10.4,"publicationDate":"2024-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://link.springer.com/content/pdf/10.1007/s11426-024-2194-0.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142249232","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Ying-Qi Zhang, Gan-Lu Qian, Yun Liu, Jia-Hui Li, Xin Hong, Zhou Xu, Bo Zhou, Long-Wu Ye
{"title":"Tandem asymmetric dearomatized functionalization reaction of phenols with Evans-ynamides enabled by divergent electrophiles","authors":"Ying-Qi Zhang, Gan-Lu Qian, Yun Liu, Jia-Hui Li, Xin Hong, Zhou Xu, Bo Zhou, Long-Wu Ye","doi":"10.1007/s11426-024-2211-y","DOIUrl":"10.1007/s11426-024-2211-y","url":null,"abstract":"<div><p>Herein, we disclose a highly regio-/chemoselective tandem asymmetric dearomatized halofunctionalization reaction of phenol-tethered ynamides with diverse electrophilic halogenation sources in a catalyst-free manner for the practical and rapid assembly of a series of halogenated spirocyclic enones. Besides, the related dearomatized selenation and protonation are also achieved, affording the corresponding selenated and protonated spirocycles in high efficiency. Moreover, the enantioselectivities of these products can be perfectly induced by Evans auxiliaries (99% ees). Significantly, this protocol not only represents the first tandem asymmetric halofunctionalization reaction of phenol derivatives, but also constitutes the first asymmetric halogenation/selenation of ynamides. Theoretical calculations indicate a remote induction model of Evans chiral auxiliary-attached keteniminium.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 2","pages":"649 - 660"},"PeriodicalIF":10.4,"publicationDate":"2024-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142249237","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":"Combating periodontitis with an ATP-responsive metal-organic framework through synergistic ion-interference-induced pyroptosis","authors":"Yuling Xu, Mengrong He, Xuechuan Hong","doi":"10.1007/s11426-024-2192-9","DOIUrl":"10.1007/s11426-024-2192-9","url":null,"abstract":"","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"67 11","pages":"3493 - 3494"},"PeriodicalIF":10.4,"publicationDate":"2024-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142518542","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}