Science China Chemistry最新文献

{"title":"Direct and rapid detection of serum amino acid and monoamine neurotransmitters to assist the diagnosis of panic disorder","authors":"Shiwen Liu,&nbsp;Xuerui Wan,&nbsp;Meng Zhao,&nbsp;Jiaqi Wang,&nbsp;Weilan Wu,&nbsp;Linlin You,&nbsp;Yonggui Yuan,&nbsp;Qian Xu,&nbsp;Rong Gao","doi":"10.1007/s11426-024-2150-5","DOIUrl":"10.1007/s11426-024-2150-5","url":null,"abstract":"<div><p>The measurement of amino acid and monoamine neurotransmitters (NTs) in serum plays a central role in the identification and monitoring of clinical panic disorder (PD). However, the strong polarity and chemical heterogeneity of NTs make direct extraction and rapid detection extremely challenging. Herein, we developed a strategy that integrated solid phase extraction based on magnetic Fe₃O₄ coated with polydopamine (Fe₃O₄@PDA) and direct analysis of mass spectrometry in real time (DART-MS) for quantification of 10 NTs. We systematically investigated the optimal conditions of this strategy to achieve good accuracy and precision. Compared with existing magnetic solid phase extraction methods for NTs detection in biological samples, this strategy could adsorb more targets while having similar adsorption efficiencies, and the total process time was reduced by an average of 69.42%. We rapidly determined the metabolic abnormality of 6 types of NTs in the serum of PD patients and demonstrated their diagnostic accuracy. In addition, an outstanding feature of PD in which tryptophan was more metabolized by the KYN pathway and the 5-hydroxytryptamine pathway was inhibited could be elucidated by this strategy. Our results highlighted the potential ability of Fe₃O₄@PDA coupled with DART-MS to assist in the clinical diagnosis of PD.\u0000</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 1","pages":"377 - 384"},"PeriodicalIF":10.4,"publicationDate":"2024-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142925472","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":"Enantioselective iridium-catalyzed allylic substitution with a Reformatsky reagent: direct construction of β-stereogenic homoallylic esters","authors":"Debasis Pal,&nbsp;Kirana D. Veeranna,&nbsp;Yuk Fai Wong,&nbsp;P. Andrew Evans","doi":"10.1007/s11426-024-2284-x","DOIUrl":"10.1007/s11426-024-2284-x","url":null,"abstract":"<div><p>The Reformatsky reagent derived from ethyl bromoacetate circumvents the challenge associated with the direct regio- and enantioselective iridium-catalyzed allylic alkylation with an unstabilized aliphatic ester enolate. Notably, this work represents the first example of using a Reformatsky reagent in a metal-allyl reaction, which permits the direct construction of enantioenriched β-stereogenic homoallylic esters without preactivation of the pronucleophile or post-reaction modification of the product (e.g., thermal decarboxylation of a 1,3-dicarbonyl). Moreover, the process allows the coupling of a broad range of sterically and electronically diverse electrophiles bearing aryl, heteroaryl and alkenyl derivatives, including the significantly more challenging alkyl-substituted allylic carbonates. The versatility of the ester product is exemplified by a series of functional group manipulations and the development of a concise and efficient enantioselective total synthesis of the natural product, (+)-descurainolide A. Finally, mechanistic studies indicate that the zinc enolate behaves as a soft nucleophile that undergoes outer-sphere alkylation.\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":"3791 - 3797"},"PeriodicalIF":10.4,"publicationDate":"2024-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142519159","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":"Thioredoxin pathway regulated live-cell synthesis of CdSe quantum dots in Saccharomyces cerevisiae","authors":"Xu Li,&nbsp;Cai-Qin Wu,&nbsp;Jia-Wei Tu,&nbsp;Juan Kong,&nbsp;Ling-Ling Yang,&nbsp;Zhi-Xiong Xie,&nbsp;Dai-Wen Pang","doi":"10.1007/s11426-024-2261-x","DOIUrl":"10.1007/s11426-024-2261-x","url":null,"abstract":"<div><p>Currently, the application of synthetic biology to artificially manipulate and utilize organisms for the synthesis of desired products such as nanomaterials with excellent fluorescence properties is attracting considerable attention. However, it is still difficult to obtain designed products efficiently due to insufficient knowledge of the biosynthetic mechanisms. The thioredoxin (TRX) and glutathione (GSH) pathways are generally conserved thiol-reductase systems that protect organisms from oxidative stress and are involved in selenium (Se) metabolism. In this study, we revealed the pivotal role of cytoplasmic TRX pathway in regulating the metabolism of Na₂SeO₃ during the live-cell synthesis of cadmium-selenium quantum dots (CdSe QDs) in <i>Saccharomyces cerevisiae</i> by regulating the expression level of genes related to TRX pathway and measuring the intracellular content of selenocysteine (SeCys). The determination of SeCys metabolism in yeast with GSH pathway-related genes deleted demonstrated that the TRX pathway played a more significant role in SeCys metabolism than GSH pathway. A 6.4-fold enhancement in the synthetic yield of CdSe QDs was achieved through the overexpression of TRX pathway-related genes, improvement of synthetic procedure, and supplementation of GSH based on the understanding of biological metabolism. Exploring the mechanism of CdSe QDs live-cell synthesis facilitates the precise manipulation of biological processes for the synthesis of inorganic nanomaterials.\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":"3851 - 3860"},"PeriodicalIF":10.4,"publicationDate":"2024-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142519149","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":"A universal strategy of multi-objective active learning to accelerate the discovery of organic electrode molecules","authors":"Jiayi Du,&nbsp;Jun Guo,&nbsp;Wei Liu,&nbsp;Ziwei Li,&nbsp;Gang Huang,&nbsp;Xinbo Zhang","doi":"10.1007/s11426-024-2163-1","DOIUrl":"10.1007/s11426-024-2163-1","url":null,"abstract":"<div><p>Organic electrode molecules hold significant potential as the next generation of cathode materials for Li-ion batteries. In this study, we have introduced a multi-objective active learning framework that leverages Bayesian optimization and non-dominated sorting genetic algorithms-II. This framework enables the selection of organic molecules characterized by high theoretical energy density and low gap (LUMO-HOMO) (LUMO, lowest unoccupied molecular orbital; HOMO, highest occupied molecular orbital). Remarkably, after only two cycles of active learning, the determination of coefficient can reach 0.962 for theoretical energy density and 0.920 for the gap with a modest dataset of 300 molecules, showcasing superior predictive capabilities. The 2,3,5,6-tetrafluorocyclohexa-2,5-diene-1,4-dione, selected by non-dominated sorting genetic algorithms-II, has been successfully applied to Li-ion batteries as cathode materials, demonstrating a high capacity of 288 mAh g⁻¹ and a long cycle life of 1,000 cycles. This outcome underscores the high reliability of our framework. Furthermore, we have also validated the universality and transferability of our framework by applying it to two additional databases, the QM9 and OMEAD. When the training dataset of the model includes at least 500 molecules, the determination of coefficient essentially reaches approximately 0.900 for four targets: gap, reduction potential, LUMO, and HOMO. Therefore, the universal framework in our work provides innovative insights applicable to other domains to expedite the screening process for target materials.\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":"3681 - 3687"},"PeriodicalIF":10.4,"publicationDate":"2024-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142519153","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":"Buried interface bridging for inverted cesium-formamidinium triiodide perovskite solar cells with long operational stability","authors":"Chenhui Zhang,&nbsp;Chunjun Liang,&nbsp;Fulin Sun,&nbsp;Ting Zhu,&nbsp;Xinghai Huang,&nbsp;Yuzhu Guo,&nbsp;Xinyu Guo,&nbsp;Kunyang Ge,&nbsp;Dan Li,&nbsp;Fangtian You,&nbsp;Zhiqun He","doi":"10.1007/s11426-024-2234-x","DOIUrl":"10.1007/s11426-024-2234-x","url":null,"abstract":"<div><p>In the field of perovskite solar cells (PSCs), the research on defects in the buried interface has been relatively limited due to its non-exposure; however, this interface significantly impacts the performance enhancement of inverted PSCs. This study employs phenylethylammonium chloride (PEACl) molecules as a buffer layer to modify the buried interface of p-i-n structured PSCs, aiming to enhance the uniformity of self-assembled monolayers (SAMs) and facilitate the uniform nucleation and growth of perovskite films on the substrate. Furthermore, the introduction of the PEACl buffer layer effectively passivates defects at the bottom of the perovskite layer and notably enhances the crystal quality of the perovskite film by mitigating residual stress, thereby reducing nonradiative recombination loss. Following these optimizations, the MA-free PSCs treated with PEACl achieve a power conversion efficiency (PCE) of 24.11%, with significant improvements in storage, thermal stability, and operational stability. Particularly noteworthy is the device’s performance in an unencapsulated state, whereas after 1,500 hours of continuous light operation stability testing, it retains 97% of its original efficiency. This study not only enriches the systematic understanding of the characteristics of the buried interface in PSCs but also contributes significantly to advancing the commercial production of perovskite photovoltaic technology.\u0000</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 1","pages":"163 - 173"},"PeriodicalIF":10.4,"publicationDate":"2024-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142925484","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":"Porous organic cages as a novel platform for second harmonic generation","authors":"Feng Shui,&nbsp;Yunqin Zhang,&nbsp;Mao Yi,&nbsp;Xiongli Liu,&nbsp;Lin Li,&nbsp;Shuo Zhang,&nbsp;Yongshen Zheng,&nbsp;Yongtao Yao,&nbsp;Qiao Zhao,&nbsp;Baiyan Li,&nbsp;Xianhe Bu","doi":"10.1007/s11426-024-2162-5","DOIUrl":"10.1007/s11426-024-2162-5","url":null,"abstract":"<div><p>Second harmonic generation (SHG) is one of the most extensively applied nonlinear optical phenomena. Compared to traditional inorganic SHG materials, organic SHG materials, including non-centrosymmetric small molecular crystals and organic polymers, have been extensively explored for SHG optics due to their advantageous properties, including high light-induced damage threshold, ultrafast response speed, high polarization ratio, wide transparency range, and elevated dielectric constant. However, in organic SHG materials, most small molecular crystals often show poor thermal stability (&lt;200 °C) due to their low molecular weight, which is an important obstacle for practical application under high temperatures. On the other hand, the difficulty in the growth of large-size crystals as well as the disorderly array of chromospheres on polymer chains associated with organic polymers have hindered their widespread application in SHG due to the requirements of processability and homogeneity. Therefore, it is significantly necessary to develop novel organic SHG material with high thermal stability, large-size crystals, excellent processability, high homogeneity, and a well SHG effect. In the contribution, we developed herein porous organic cages (POCs) as a novel platform for SHG optics. Thanks to its inherent macromolecular composition and zero-dimensional discrete structures, POCs can not only solve the instability problem of small molecule crystals but also overcome the drawbacks in growing large-size crystals for organic polymer. The obtained two POCs with chiral asymmetric centers (CPOC-R-5 and CPOC-S-7) display advantageous features for SHG optics including well SHG performance, large-size crystal (5 mm×3 mm×1 mm), high thermal stability (⩾250 °C), wide transparency window (750–2,000 nm) and high polarization ratio (up to 94.5%). This work thus develops POCs as a new platform toward the construction of organic NLO materials with the potential application in sorts of SHG optics.\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":"3669 - 3674"},"PeriodicalIF":10.4,"publicationDate":"2024-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://link.springer.com/content/pdf/10.1007/s11426-024-2162-5.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142519151","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":"Mainchain conformation ordering self-assembly tailored room temperature phosphorescence emission","authors":"Yuzhu Li,&nbsp;Yumeng Gao,&nbsp;Feng Tian,&nbsp;Yu Wang,&nbsp;Yuan Yao,&nbsp;Shaoliang Lin,&nbsp;Xiang Ma,&nbsp;Binbin Xu","doi":"10.1007/s11426-024-2147-x","DOIUrl":"10.1007/s11426-024-2147-x","url":null,"abstract":"<div><p>Developing organic room-temperature phosphorescence (RTP) materials with a wide range of tunable-emission is significant in expanding the applications of RTP materials. Herein, we rationally designed amphiphilic alternating copolymers poly(1,2-bis(4-alkoxyphenyl)ethane-1,2-dione-<i>alt</i>-(ethylene glycol)_<i>x</i>) (P(Bz-<i>alt</i>-EG_<i>x</i>)) that combined the advantage of alternating benzil and EG_<i>x</i> skeleton, and tunable mainchain conformation. Through a mainchain conformation ordering assembly (COA) process, P (Bz-<i>alt</i>-EG_<i>x</i>) self-assembled into well-defined platelets, and such assemblies emitted blue RTP at ca. 425 nm due to the ordered folded-chain conformation and confined microenvironment. In contrast, traditional self-assembly (TA) of P(Bz-<i>alt</i>-EG_<i>x</i>) obtained less ordered aggregates, such as asymmetric worms, vesicles, and rod-like micelles. The resultant less ordered aggregates exhibited yellow-green RTP at ca. 550 nm. The wide-tuning RTP emission in solution (between blue and yellow-green, over 125 nm) is realized using the P(Bz-<i>alt</i>-EG_<i>x</i>) alternating copolymers under the treatment of different self-assembly conditions. This study uncovers a new strategy to tailor the RTP emission through different self-assembly pathways and holds great promise for the fabrication of advanced optical materials.\u0000</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 1","pages":"329 - 336"},"PeriodicalIF":10.4,"publicationDate":"2024-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142925485","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":"Tandem electrocatalysis for CO2 reduction to multi-carbons","authors":"Xindi Li,&nbsp;Tianxiang Yan,&nbsp;Yichen Meng,&nbsp;Zhanpeng Liang,&nbsp;Tianying Zhang,&nbsp;Haoyuan Chi,&nbsp;Ziting Fan,&nbsp;Yifan Jin,&nbsp;Haoran Zhang,&nbsp;Sheng Zhang","doi":"10.1007/s11426-024-2144-0","DOIUrl":"10.1007/s11426-024-2144-0","url":null,"abstract":"<div><p>The rising CO₂ concentration in the atmosphere due to extensive use of fossil fuels has led to serious climate and environmental issues. One efficient solution is that CO₂ capture from industrial emissions followed its conversion into value-added chemicals driven by renewable energies. CO₂ electroreduction (CO₂RR) features a green and sustainable fashion towards effective CO₂ conversion, but still suffers from low multi-carbon selectivity and yield. Considering the pivotal role of CO intermediate in C–C coupling to multi-carbon formation, tandem CO₂RR systems with separated CO generation and consumption components could facilitate the coupling between *CO-based intermediates to energy-intensive multi-carbons by manipulating CO diffusion and surface coverage. In this aspect, we comprehensively reviewed the design principles of tandem systems for CO₂ electroreduction reaction. The chemistry behind the C–C coupling regarding to their distribution and diffusion was initially introduced, which was followed by achievements on tandem architectures, from catalysts, electrodes to systems. Future directions and perspectives on advanced tandem system designs for CO₂RR were discussed at the end. This review contributes to the understanding of structure-performance correlations in tandem catalysis and helps guide the effective collection of multi-carbons of high-yield and high-selectivity.\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":"3631 - 3651"},"PeriodicalIF":10.4,"publicationDate":"2024-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142519152","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":"A MOF built on 8-connected Y3 nodes demonstrates simultaneous reverse adsorptive separation: ethane over ethylene and propane over propylene","authors":"Lu-Lu Ma,&nbsp;Jiaqi Liu,&nbsp;Kang Zhou,&nbsp;Zixuan Cao,&nbsp;Jiafeng Miao,&nbsp;Guo-Ping Yang,&nbsp;Yao-Yu Wang,&nbsp;Jing Li,&nbsp;Hao Wang","doi":"10.1007/s11426-024-2185-8","DOIUrl":"10.1007/s11426-024-2185-8","url":null,"abstract":"<div><p>Selective adsorption of paraffins over olefins (mostly C2 and C3) by porous solids could offer tremendous advantages for the purification of olefins, which is, however, challenging as it has stringent requirements on the pore dimensions and pore surface chemistry of the adsorbent. We report here a metal-organic framework (MOF) with novel topology, Y₃(<i>μ</i>₃-OH)(TCMPB)₂ (denoted as HIAM-316, TCMPB⁴⁻ = 1,2,4,5-tetra(4-carboxy-3-methylphenyl)benzene), which shows reversed separation of C₂H₆/C₂H₄ and C₃H₈/C₃H₆ simultaneously. The ideal adsorbed solution theory (IAST) selectivities for equimolar binary mixtures of C₂H₆/C₂H₄ and C₃H₈/C₃H₆ were calculated to be 1.67 and 1.23 at 1 bar and 298 K for HIAM-316. Its capability of removing paraffines from paraffin/olefin mixtures is validated by breakthrough measurements. Molecular simulations reveal that the preferential adsorption of paraffins over olefins by HIAM-316 may be attributed to the abundant carboxylate oxygen atoms along its channel.\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":"3657 - 3661"},"PeriodicalIF":10.4,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142519050","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":"Prospects and challenges in electrochemical nitrogen activation for ammonia synthesis","authors":"Xianbiao Fu,&nbsp;Ib Chorkendorff","doi":"10.1007/s11426-024-2129-6","DOIUrl":"10.1007/s11426-024-2129-6","url":null,"abstract":"","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"67 11","pages":"3510 - 3514"},"PeriodicalIF":10.4,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://link.springer.com/content/pdf/10.1007/s11426-024-2129-6.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142519049","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}