Chemical Science最新文献_第10页

Interfacial engineering of Ru-RuSb₂ for enhanced activity and stability towards alkaline hydrogen oxidation reaction. Ru-RuSb2增强碱性氢氧化反应活性和稳定性的界面工程研究。

IF 7.6 1区化学

Chemical Science Pub Date : 2025-07-10 DOI: 10.1039/d5sc03850b

Chaoyi Yang, Zihao Dai, Jianchao Yue, Wei Luo

{"title":"Interfacial engineering of Ru-RuSb2 for enhanced activity and stability towards alkaline hydrogen oxidation reaction.","authors":"Chaoyi Yang, Zihao Dai, Jianchao Yue, Wei Luo","doi":"10.1039/d5sc03850b","DOIUrl":"10.1039/d5sc03850b","url":null,"abstract":"Although Ru has been regarded as the key candidate to replace Pt in alkaline hydrogen oxidation reaction (HOR), the substandard stability owing to its easy oxidation seriously impacts its practical application. In this work, we report the construction of a Ru-RuSb2 heterostructure, showing excellent performance and stability towards alkaline HOR. Owing to the difference in the work functions of Ru and RuSb2, the charge transfer induced by the build-in electric field modifies the electron distribution on the surface, enhancing the OH adsorption on the heterostructure. Moreover, the connectivity of the hydrogen bonding network is promoted with the inducing of OH species, which thereby leads to elevated proton transfer and accelerated HOR process, presenting a mass activity (j k,m) of 2.098 mA μg-1 at 50 mV, which is 6-fold and 20-fold higher than those of Pt/Ccom and Ru/NC, respectively. Owing to the change of the OH adsorption sites on Sb and the rapid HOR process on the surface, the pace of the oxidation on Ru of the heterostructure during the reaction largely slows down, contributing to the outstanding stability with only 2.59% decline in the activity.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":" ","pages":""},"PeriodicalIF":7.6,"publicationDate":"2025-07-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12264760/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144658572","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}

引用次数: 0

Europium probe binding to serum albumin and α-1-AGP, key importance of configuration, charge and size complementarity 铕探针结合血清白蛋白和α-1-AGP，构型、电荷和大小互补至关重要

IF 8.4 1区化学

Chemical Science Pub Date : 2025-07-08 DOI: 10.1039/d5sc03017j

Huishan Li, Lok Wan Ng, Dominic J. Black, Wei Han, Robert Pal, David Parker

引用次数: 0

Effective Generation of Heavy-Atom-Free Triplet Photosensitizers Containing Multiple Intersystem Crossing Mechanisms Based on Deep Learning 基于深度学习的含多系统交叉机制的重原子无三重态光敏剂的有效生成

IF 8.4 1区化学

Chemical Science Pub Date : 2025-07-08 DOI: 10.1039/d5sc03192c

Kepeng Chen, Xiaoting Zhang, Jike Wang, Dan Li, Tingjun Hou, Wenbo Yang, Yu Kang

{"title":"Effective Generation of Heavy-Atom-Free Triplet Photosensitizers Containing Multiple Intersystem Crossing Mechanisms Based on Deep Learning","authors":"Kepeng Chen, Xiaoting Zhang, Jike Wang, Dan Li, Tingjun Hou, Wenbo Yang, Yu Kang","doi":"10.1039/d5sc03192c","DOIUrl":"https://doi.org/10.1039/d5sc03192c","url":null,"abstract":"Photodynamic therapy (PDT) is a clinically approved therapeutic modality that has demonstrated significant potential for cancer treatment, and triplet photosensitizers (PSs) play a key role in its efficacy. Despite deep learning has emerged as a next-generation tool for material discovery, existing methods mainly target a limited subset of triplet PSs, such as thermally activated delayed fluorescence (TADF) materials, neglecting the critical intersystem crossing (ISC) between high-lying singlet and triplet states (ΔESnTn). To overcome this limitation, we compiled a comprehensive dataset (~1.90 × 109) of triplet PSs encompassing various ISC mechanisms. Then, we proposed a novel strategy that incorporates two models: a fragment-based model (Frag-MD) and a character-based model (MD), both integrating a conditional transformer, recurrent neural networks, and reinforcement learning. In silico experiments reveal that the Frag-MD model outperforms the MD model in generating larger conjugated motifs with higher average ring numbers and atom counts; while the MD model generates twice as many unique motifs and excels in novelty and diversity, as evaluated by conditional and MOSES metrics. Therefore, our approach is highly effective for modifying conjugated motifs and designing novel triplet PSs. Notably, recently reported high-efficiency triplet PSs have been re-identified through ablation experiments using our proposed models, which target ΔESnTn and significantly outperform traditional baselines, achieving a prediction accuracy of 73% versus 4%. Our approach holds the potential to establish a new paradigm for discovering novel PSs applicable in PDT.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"21 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-07-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144577807","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}

引用次数: 0

Harnessing emergent multiple scattering resonances in a photonic glass structure for photoelectrochemical energy conversion 利用光子玻璃结构中涌现的多重散射共振进行光电化学能量转换

IF 8.4 1区化学

Chemical Science Pub Date : 2025-07-08 DOI: 10.1039/d5sc02916c

Ashlyn G. DesCarpentrie, Robert H. Coridan

{"title":"Harnessing emergent multiple scattering resonances in a photonic glass structure for photoelectrochemical energy conversion","authors":"Ashlyn G. DesCarpentrie, Robert H. Coridan","doi":"10.1039/d5sc02916c","DOIUrl":"https://doi.org/10.1039/d5sc02916c","url":null,"abstract":"Light trapping nanostructures are often necessary to improve carrier collection yields in semiconductor photoelectrodes with intrinsically poor electron transport. Photonic crystal templates can generate tailorable light trapping via periodic and precise nanostructure, though this is not a scalable strategy for photoelectrochemical (PEC) applications. It is therefore critical to identify alternative mechanisms for light trapping that tolerate disorder. Light trapping in disordered media is generated by the diffusive transport caused by multiple scattering. In some cases, multiple scattering can generate resonances that resemble those observed in photonic crystals. While resonant multiple scattering is a disorder tolerant light trapping mechanism, it is unclear if the effect is sufficiently adaptable, or even useful, for PEC applications. Here, we describe a photonic omission glass, a nanostructure that can controllably induce resonances in multiple scattering transport. We characterized the emergence of these resonances after coating a disordered SiO2 colloidal structure with a layer of TiO2, which functions both as dielectric contrast and as a light absorbing semiconductor. We show in finite element simulations and spectroscopic characterization that the resonant multiple scattering effect improves light trapping near the interface between the structure and the bulk electrolyte. This effect, coupled with the increased electrochemically active surface area, results in a hierarchically structured TiO2 photoanode with orders of magnitude higher photocurrents compared to an equivalent planar photoanode for PEC reactions such as alkaline water oxidation. We show that controlling this resonant multiple scattering effect can be advantageous for improving PEC energy conversion in disordered photoelectrodes.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"31 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-07-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144577808","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}

引用次数: 0

Identification, occurrence and prevention of aspartimide-related byproducts in chemical protein synthesis 化学蛋白质合成中阿斯巴胺相关副产物的鉴定、发生及预防

IF 8.4 1区化学

Chemical Science Pub Date : 2025-07-08 DOI: 10.1039/d5sc03824c

Vincent Aucagne, El hadji Cisse

{"title":"Identification, occurrence and prevention of aspartimide-related byproducts in chemical protein synthesis","authors":"Vincent Aucagne, El hadji Cisse","doi":"10.1039/d5sc03824c","DOIUrl":"https://doi.org/10.1039/d5sc03824c","url":null,"abstract":"Formation of a five-membered ring aspartimide through the attack of a backbone amide to the side chain of aspartate and asparagine residues is a long-known side-reaction in solid phase peptide synthesis, and is also associated with in vivo protein ageing and instability of purified proteins. Conversely, its possible occurrence during chemical ligation-based protein synthesis, in particular when using the gold-standard reaction NCL (native chemical ligation), is dubious. We herein report a systematic study which demonstrates that the prevalence of this side-reaction may have been overlooked, due to the difficulty to identify it through standard HPLC analytical methods, but also the in situ conversion of aspartimide into other byproducts, having the same molecular mass as the parent aspartate residue. We show that the formation of aspartimide and derived byproducts can be limited by adopting \"good NCL practices\", which involve restricting the ligation temperature and reaction times, as well as replacing the commonly used phosphate buffer with HEPES. However, the efficiency of such precautions is expected to vary considerably depending on the sequence of the target protein, and the amount of byproducts is expected to grow with the length of the target protein, as a result of the number of NCL reactions and potential aspartimide hotspots. To overcome such limitations, we developed a novel straightforward and potentially generally applicable methodology based on the temporary protection of the backbone nitrogen by a 2-(4-aminobutanoyloxy)-4-methoxybenzyl (GABA-Hmb) group. This strategy was validated by the byproduct-free synthesis of SUMO-2 and a SUMOylated peptide mimic.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"93 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-07-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144577809","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}

引用次数: 0

Regulating the donor number of solvents for long-cycle anode-free lithium metal batteries 长循环无阳极锂金属电池溶剂用量的调节

IF 8.4 1区化学

Chemical Science Pub Date : 2025-07-08 DOI: 10.1039/d5sc02399h

Yining Zhao, Shaopeng Li, Yahui Li, Shu Xu, Lingtong Zhu, Hui Dou, Xiaogang Zhang

{"title":"Regulating the donor number of solvents for long-cycle anode-free lithium metal batteries","authors":"Yining Zhao, Shaopeng Li, Yahui Li, Shu Xu, Lingtong Zhu, Hui Dou, Xiaogang Zhang","doi":"10.1039/d5sc02399h","DOIUrl":"https://doi.org/10.1039/d5sc02399h","url":null,"abstract":"Anode-free lithium-metal batteries (AFLMBs) are one of the up-and-coming high-energy-density battery systems because they eliminate the need for conventional graphite electrodes or excess lithium metal anodes (LMAs). However, AFLMBs have serious problems of low coulombic efficiencies (CEs) and poor cycle stability. Herein, this study proposes a local high-concentration electrolyte (LHCE) based on donor number (DN) modulation, which achieves stable dissolution of LiNO3 and an anion-enhanced solvation structure through the synergistic action of a high DN solvent (Tetraglyme, G4) and an ultra-low DN diluent (1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropyl ether, TTE). The design addresses the core challenges of low CEs and poor cycling stability in AFLMBs due to the lack of lithium source. Computational and experimental results show that regulating the DN value of the solvent significantly reduces the Li+ desolvation energy and forms an inorganic-rich solid electrolyte interphase (SEI), which guides the uniform deposition of Li. The electrolyte achieves a high CE (about 99.0%) and long cycle life (1400 h). Based on this, AFLMB maintains 86.3% capacity after 50 cycles, far exceeding the 25-cycle life of conventional carbonate electrolytes (CCE).","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"21 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-07-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144577818","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}

引用次数: 0

Unlocking Inverted Singlet-Triplet Gap in Alternant Hydrocarbons with Heteroatoms 杂原子交替碳氢化合物中反向单重态-三重态间隙的解锁

IF 8.4 1区化学

Chemical Science Pub Date : 2025-07-08 DOI: 10.1039/d5sc02309b

Atreyee Majumdar, Surajit Das, Raghunathan Ramakrishnan

引用次数: 0

Bis(amidophenolate)-supported pnictoranides: Lewis acid-induced electromerism in a bismuth complex 双（氨基酚酸酯）支持的pnictoranides：铋配合物中路易斯酸诱导的电聚合

IF 8.4 1区化学

Chemical Science Pub Date : 2025-07-08 DOI: 10.1039/d5sc03374h

Simon B. H. Karnbrock, Jan F. Köster, Isabelle Becker, Christopher Golz, Franc Meyer, Martí Gimferrer, Manuel Alcarazo

引用次数: 0

Correction: Water entropy at the threonine-rich surface of antifreeze and ice-nucleating proteins: small changes make a big difference 更正：防冻剂和冰核蛋白富含苏氨酸表面的水熵：微小的变化会产生巨大的差异