Jiale Wei, Jing Jiang, Chuqi Li, Guo Wang, Jiayao Wulan, Huan Yang, Fangxu Shen, Daixin Ye, Kai Li, Xianchan Li, Yuqing Lin
Nicotinamide adenine dinucleotide (NADH), a crucial biomarker for cellular redox homeostasis, is intrinsically linked to mitochondrial function and neurodegenerative diseases. However, electrochemical detection of intracellular NADH faces dual challenges: low abundance and biofouling, as well as high overpotential. Herein, we designed a hydrogen-bond-assisted meta-nitrogen/oxygen co-doped graphyne (3NGYO) nanoelectrode for high-performance NADH sensing. Precise tri-N doping in graphyne (3NGY) generates sp2-N atoms associated with hydrogen atoms. Specifically, pyrrolic N-H forms a 2.502 Å N-H⋯O[double bond, length as m-dash]P hydrogen bond with NADH's PO4 groups, boosting adsorption energy to -5.48 eV and reducing NADH oxidation potential to 0 V. This achieves a 59-fold higher catalytic current response compared to pristine graphyne. Subsequent acid oxidation introduces oxygen-containing functional groups (e.g., -COOH, C[double bond, length as m-dash]O), increasing hydrophilicity (contact angle: 54.0°) and anti-fouling performance (80% current retention after 2 h BSA exposure). Electrodeposited 3NGYO nanotips attain a sensitivity of 0.419 pA µM-1 and a linear range of 0-20 µM at +0.2 V vs. Ag/AgCl. Real-time amperometry in SH-SY5Y cells demonstrates that 1-methyl-4-phenylpyridinium (MPP+)-induced mitochondrial dysfunction triggers NADH release. In contrast, hydrogen sulfide (H2S) pretreatment reduces NADH leakage by 95.4%, correlating with suppressed calcium ion (Ca2+) influx and reactive oxygen species (ROS) generation. This work provides a tool for studying mitochondrial dysfunction and establishes a new paradigm for in situ electrocatalytic biosensing.
烟酰胺腺嘌呤二核苷酸（Nicotinamide adenine dinucleotide， NADH）是细胞氧化还原稳态的重要生物标志物，与线粒体功能和神经退行性疾病有内在联系。然而，细胞内NADH的电化学检测面临着双重挑战：低丰度和生物污染，以及高过电位。在此，我们设计了一种氢键辅助的间氮/氧共掺杂石墨炔（3NGYO）纳米电极，用于高性能的NADH传感。在石墨炔（3NGY）中精确掺杂三氮，生成与氢原子结合的sp2-N原子。具体来说，吡咯烷N-H与NADH的PO4基团形成2.502 Å N-H⋯O[双键，长度为m-dash]P氢键，将吸附能提高到-5.48 eV，并将NADH氧化电位降低到0 V。与原始石墨炔相比，这实现了59倍高的催化电流响应。随后的酸氧化引入了含氧官能团（例如，-COOH， C[双键，长度为m-dash]O），增加了亲水性（接触角：54.0°）和防污性能（暴露于BSA 2小时后电流保留80%）。电沉积的3NGYO纳米针尖在+0.2 V vs. Ag/AgCl下的灵敏度为0.419 pAµM-1，线性范围为0-20µM。SH-SY5Y细胞的实时电流测定表明，1-甲基-4-苯基吡啶（MPP+）诱导的线粒体功能障碍触发NADH释放。相比之下，硫化氢（H2S）预处理减少了95.4%的NADH泄漏，这与抑制钙离子（Ca2+）内流和活性氧（ROS）的产生有关。这项工作为研究线粒体功能障碍提供了工具，并建立了原位电催化生物传感的新范式。
{"title":"Hydrogen-bond-assisted meta-nitrogen-doped graphyne enables real-time electrocatalytic NADH tracking in single cells.","authors":"Jiale Wei, Jing Jiang, Chuqi Li, Guo Wang, Jiayao Wulan, Huan Yang, Fangxu Shen, Daixin Ye, Kai Li, Xianchan Li, Yuqing Lin","doi":"10.1039/d5sc08242k","DOIUrl":"10.1039/d5sc08242k","url":null,"abstract":"<p><p>Nicotinamide adenine dinucleotide (NADH), a crucial biomarker for cellular redox homeostasis, is intrinsically linked to mitochondrial function and neurodegenerative diseases. However, electrochemical detection of intracellular NADH faces dual challenges: low abundance and biofouling, as well as high overpotential. Herein, we designed a hydrogen-bond-assisted <i>meta</i>-nitrogen/oxygen co-doped graphyne (3NGYO) nanoelectrode for high-performance NADH sensing. Precise tri-N doping in graphyne (3NGY) generates sp<sup>2</sup>-N atoms associated with hydrogen atoms. Specifically, pyrrolic N-H forms a 2.502 Å N-H⋯O[double bond, length as m-dash]P hydrogen bond with NADH's PO<sub>4</sub> groups, boosting adsorption energy to -5.48 eV and reducing NADH oxidation potential to 0 V. This achieves a 59-fold higher catalytic current response compared to pristine graphyne. Subsequent acid oxidation introduces oxygen-containing functional groups (<i>e.g.</i>, -COOH, C[double bond, length as m-dash]O), increasing hydrophilicity (contact angle: 54.0°) and anti-fouling performance (80% current retention after 2 h BSA exposure). Electrodeposited 3NGYO nanotips attain a sensitivity of 0.419 pA µM<sup>-1</sup> and a linear range of 0-20 µM at +0.2 V <i>vs.</i> Ag/AgCl. Real-time amperometry in SH-SY5Y cells demonstrates that 1-methyl-4-phenylpyridinium (MPP<sup>+</sup>)-induced mitochondrial dysfunction triggers NADH release. In contrast, hydrogen sulfide (H<sub>2</sub>S) pretreatment reduces NADH leakage by 95.4%, correlating with suppressed calcium ion (Ca<sup>2+</sup>) influx and reactive oxygen species (ROS) generation. This work provides a tool for studying mitochondrial dysfunction and establishes a new paradigm for <i>in situ</i> electrocatalytic biosensing.</p>","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":" ","pages":""},"PeriodicalIF":7.4,"publicationDate":"2026-01-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12794285/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145965753","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}
Artemijs Krimovs, Dominic J. Black, Aileen Congreve, Robert Pal
A novel arylalkynylpyridine-sensitised nine coordinate quasi-C3 symmetric all carboxylate donor europium(III) complex (EuL) possessing exceptionally high circularly polarised brightness in both ΔJ = 1 and ΔJ = 2 transitions was prepared and tested in spin-coated solid-state PMMA thin films. The authentication of the circularly polarised luminescence (CPL) layer was successfully performed using CPL photography (CPLP) and enantioselective differential chiral contrast (EDCC) imaging for both transitions simultaneously using appropriate band pass filters. The effect of reflective properties of different thin film substrate materials on the recorded chiral contrast was quantified using the newly introduced CPLP dissymmetry factor (gCPLP) which compared to the average dissymmetry factor values obtained using a photo elastic modulator (PEM) based CPL spectrometer. Circularly polarised brightness (CPB) of ΔJ = 2 (590 mol−1 dm3 cm−1 at 607 nm) was the highest ever reported and that of ΔJ = 1 (307 mol−1 dm3 cm−1 at 596 nm) was third best across other CPL-active materials with reported CPB. This makes EuL the best candidate for next-generation CPL-active multi-tier ‘chameleon security inks’.
{"title":"Complete stereochemical control to unlock monosign circularly polarised luminescence with superior circularly polarised brightness for chameleon security inks","authors":"Artemijs Krimovs, Dominic J. Black, Aileen Congreve, Robert Pal","doi":"10.1039/d5sc05303j","DOIUrl":"https://doi.org/10.1039/d5sc05303j","url":null,"abstract":"A novel arylalkynylpyridine-sensitised nine coordinate quasi-<em>C</em><small><sub>3</sub></small> symmetric all carboxylate donor europium(<small>III</small>) complex (EuL) possessing exceptionally high circularly polarised brightness in both Δ<em>J</em> = 1 and Δ<em>J</em> = 2 transitions was prepared and tested in spin-coated solid-state PMMA thin films. The authentication of the circularly polarised luminescence (CPL) layer was successfully performed using CPL photography (CPLP) and enantioselective differential chiral contrast (EDCC) imaging for both transitions simultaneously using appropriate band pass filters. The effect of reflective properties of different thin film substrate materials on the recorded chiral contrast was quantified using the newly introduced CPLP dissymmetry factor (<em>g</em><small><sub>CPLP</sub></small>) which compared to the average dissymmetry factor values obtained using a photo elastic modulator (PEM) based CPL spectrometer. Circularly polarised brightness (CPB) of Δ<em>J</em> = 2 (590 mol<small><sup>−1</sup></small> dm<small><sup>3</sup></small> cm<small><sup>−1</sup></small> at 607 nm) was the highest ever reported and that of Δ<em>J</em> = 1 (307 mol<small><sup>−1</sup></small> dm<small><sup>3</sup></small> cm<small><sup>−1</sup></small> at 596 nm) was third best across other CPL-active materials with reported CPB. This makes EuL the best candidate for next-generation CPL-active multi-tier ‘chameleon security inks’.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"19 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-01-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145962209","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}
The rise of artificial intelligence (AI) has taken machine learning (ML) in molecular design to a new level. As ML increasingly relies on complex deep learning frameworks, the inability to understand predictions of black-box models has become a topical issue. Consequently, there is strong interest in the field of explainable AI (XAI) to bridge the gap between black-box models and the acceptance of their predictions, especially at interfaces with experimental disciplines. Therefore, XAI methods must go beyond extracting learning patterns from ML models and present explanations of predictions in a human-centered, transparent, and interpretable manner. In this Perspective, we examine current challenges and opportunities for XAI in molecular design and evaluate the benefits of incorporating domain-specific knowledge into XAI approaches for model refinement, experimental design, and hypothesis testing. In this context, we also discuss the current limitations in evaluating results from chemical language models that are increasingly used in molecular design and drug discovery.
{"title":"Explainable artificial intelligence for molecular design in pharmaceutical research","authors":"Alec Lamens, Jürgen Bajorath","doi":"10.1039/d5sc08461j","DOIUrl":"https://doi.org/10.1039/d5sc08461j","url":null,"abstract":"The rise of artificial intelligence (AI) has taken machine learning (ML) in molecular design to a new level. As ML increasingly relies on complex deep learning frameworks, the inability to understand predictions of black-box models has become a topical issue. Consequently, there is strong interest in the field of explainable AI (XAI) to bridge the gap between black-box models and the acceptance of their predictions, especially at interfaces with experimental disciplines. Therefore, XAI methods must go beyond extracting learning patterns from ML models and present explanations of predictions in a human-centered, transparent, and interpretable manner. In this Perspective, we examine current challenges and opportunities for XAI in molecular design and evaluate the benefits of incorporating domain-specific knowledge into XAI approaches for model refinement, experimental design, and hypothesis testing. In this context, we also discuss the current limitations in evaluating results from chemical language models that are increasingly used in molecular design and drug discovery.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"27 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-01-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145949956","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}
Shuili Liu, Xingji Liu, Xiu Gu, Shicheng Dong, Nan Huang, Lei Shi, Jun Jiang
Photocatalytic heterogeneous organic transformation represents an ecofriendly and sustainable method for addressing persistent energy and environmental challenges. Conjugated porous polymer (CPP)-based materials have recently emerged as promising photocatalysts for diverse organic transformations, offering a sustainable alternative to homogeneous systems reliant on precious inorganic or organic dyes. Herein, we designed two pyrene-based CPPs for visible-light photocatalysis, featuring fluoro- or methyl-substituted fluorenes as distinct units. These CPPs act as metal-free, visible-light-activated, reusable heterogeneous photocatalysts for synthesizing benzofused oxa-heterocycles via photooxidized [4 + 2] and [3 + 2] cycloadditions of phenols with alkenes. Notably, DFT calculations demonstrate that the fluoro-block CPP with its larger dipole moment can achieve more efficient photoinduced charge separation, due to the stronger electron-attractive force. Consequently, FF-Py-CPP exhibited superior photocatalytic activity compared to MF-Py-CPP, achieving excellent yields, high diastereoselectivity, and good recyclability in the syntheses of chromanes and dihydrobenzofuran.
{"title":"Pyrene-based conjugated porous polymers as photocatalysts for oxidative cycloaddition of phenols","authors":"Shuili Liu, Xingji Liu, Xiu Gu, Shicheng Dong, Nan Huang, Lei Shi, Jun Jiang","doi":"10.1039/d5sc08900j","DOIUrl":"https://doi.org/10.1039/d5sc08900j","url":null,"abstract":"Photocatalytic heterogeneous organic transformation represents an ecofriendly and sustainable method for addressing persistent energy and environmental challenges. Conjugated porous polymer (CPP)-based materials have recently emerged as promising photocatalysts for diverse organic transformations, offering a sustainable alternative to homogeneous systems reliant on precious inorganic or organic dyes. Herein, we designed two pyrene-based CPPs for visible-light photocatalysis, featuring fluoro- or methyl-substituted fluorenes as distinct units. These CPPs act as metal-free, visible-light-activated, reusable heterogeneous photocatalysts for synthesizing benzofused oxa-heterocycles <em>via</em> photooxidized [4 + 2] and [3 + 2] cycloadditions of phenols with alkenes. Notably, DFT calculations demonstrate that the fluoro-block CPP with its larger dipole moment can achieve more efficient photoinduced charge separation, due to the stronger electron-attractive force. Consequently, FF-Py-CPP exhibited superior photocatalytic activity compared to MF-Py-CPP, achieving excellent yields, high diastereoselectivity, and good recyclability in the syntheses of chromanes and dihydrobenzofuran.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"47 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-01-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145955823","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}
As the sole renewable source of organic carbon, biomass is indispensable to the green transition, offering both abundance and carbon neutrality. The biomass-derived platform molecule, 5-hydroxymethylfurfural (HMF), can be valorized into various high-value chemicals via oxidation. Most notably, 2,5-furandicarboxylic acid (FDCA) has emerged as a crucial sustainable alternative to fossil-based terephthalic acid for polyester production. This review provides a comprehensive analysis of the electrocatalytic oxidation of HMF to FDCA. We begin by dissecting the reaction pathways and mechanisms to clarify key kinetic steps and current bottlenecks. To establish benchmarks for the field, we summarize standard evaluation metrics that enable rigorous comparison among disparate studies. The review then systematically categorizes diverse catalyst systems and engineering strategies, with a specific focus on how reaction parameters (pH, electrolyte composition, and applied potential) dictate product selectivity. Concluding with a forward-looking perspective, we propose future directions to accelerate the development of efficient, controllable, and low-cost technologies for FDCA production.
{"title":"Electrosynthesis of 2,5-Furandicarboxylic Acid from 5-Hydroxymethylfurfural: Mechanisms, Advanced Catalysts, and Reaction Microenvironments","authors":"Jiacheng Zhang, Siping Wang, Jiaqing Liu, Jiayi Chen, Guigang Zhang, Yidong Hou, Meifang Zheng, Sibo Wang, Xue Feng Lu","doi":"10.1039/d5sc09723a","DOIUrl":"https://doi.org/10.1039/d5sc09723a","url":null,"abstract":"As the sole renewable source of organic carbon, biomass is indispensable to the green transition, offering both abundance and carbon neutrality. The biomass-derived platform molecule, 5-hydroxymethylfurfural (HMF), can be valorized into various high-value chemicals via oxidation. Most notably, 2,5-furandicarboxylic acid (FDCA) has emerged as a crucial sustainable alternative to fossil-based terephthalic acid for polyester production. This review provides a comprehensive analysis of the electrocatalytic oxidation of HMF to FDCA. We begin by dissecting the reaction pathways and mechanisms to clarify key kinetic steps and current bottlenecks. To establish benchmarks for the field, we summarize standard evaluation metrics that enable rigorous comparison among disparate studies. The review then systematically categorizes diverse catalyst systems and engineering strategies, with a specific focus on how reaction parameters (pH, electrolyte composition, and applied potential) dictate product selectivity. Concluding with a forward-looking perspective, we propose future directions to accelerate the development of efficient, controllable, and low-cost technologies for FDCA production.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"18 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-01-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145955827","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}
The environmental implications of all photovoltaic (PV) technologies should be rigorously assessed throughout their entire lifecycle. Perovskite PVs have emerged as a transformative innovation, challenging the dominance of conventional silicon PVs, with numerous companies now commercializing this promising technology. While efforts to enhance the efficiency and longevity of perovskite PVs are crucial, it is equally important to develop sustainable and cost-effective methods for disposing of waste perovskite solar panels, especially given their significant content of water-soluble lead ions. In this study, we explore the feasibility of employing incineration to process degraded flexible perovskite solar modules. We analyze the decomposition byproducts and their potential environmental impacts. By implementing careful management of hazardous decomposition products, we demonstrate that incineration can serve as a sustainable and economical solution for the disposal of waste perovskite solar modules, offering valuable insights for the future handling of these materials.
{"title":"Thermal decomposition behavior and sustainable recycling of flexible perovskite solar modules","authors":"Xiaoyu Shi, Yangyang Liu, Tianxiao Liu, Siwei Luo, Feifei Wang, Shangshang Chen","doi":"10.1039/d5sc07083j","DOIUrl":"https://doi.org/10.1039/d5sc07083j","url":null,"abstract":"The environmental implications of all photovoltaic (PV) technologies should be rigorously assessed throughout their entire lifecycle. Perovskite PVs have emerged as a transformative innovation, challenging the dominance of conventional silicon PVs, with numerous companies now commercializing this promising technology. While efforts to enhance the efficiency and longevity of perovskite PVs are crucial, it is equally important to develop sustainable and cost-effective methods for disposing of waste perovskite solar panels, especially given their significant content of water-soluble lead ions. In this study, we explore the feasibility of employing incineration to process degraded flexible perovskite solar modules. We analyze the decomposition byproducts and their potential environmental impacts. By implementing careful management of hazardous decomposition products, we demonstrate that incineration can serve as a sustainable and economical solution for the disposal of waste perovskite solar modules, offering valuable insights for the future handling of these materials.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"20 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145947493","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}
To overcome the limited environmental stability of organic semi-transparent photovoltaic (STPV) devices, developing robust inorganic thin-film absorbers has become a critical research focus. Antimony selenide (Sb2Se3), with its Q1D crystal structure, excellent optoelectronic properties, and mechanical flexibility, is a promising candidate for STPV applications. However, thinning the absorber to enhance visible transmittance often degrades crystallinity, weakens preferred orientation, and increases defect density. Here, we present a dual-pathway device-engineering strategy that integrates KOH-assisted chemical-bath thinning of the CdS buffer layer with rapid thermal evaporation combined with magnetron sputtering of active selenium (Se). The introduced active Se atoms effectively reorganize molecular chains within a confined crystallization space, enhancing crystalline quality and promoting vertical [hk1] orientation. Simultaneously, Se doping passivates selenium vacancies and suppresses deep-level trap states, thereby improving carrier transport and reducing nonradiative recombination. Employing this strategy, we demonstrate for the first time an ultrathin Sb2Se3 STPV device with a total functional layer thickness of only 80 nm just one-seventh the thickness of conventional devices—achieving an efficiency of 7.02%, retaining 93% of that of thicker counterparts while maintaining an optical transparency exceeding 20%. This work establishes a practical route to simultaneously balance transparency and efficiency in inorganic STPV devices and underscores the potential of Sb2Se3 as a high-performance absorber for next-generation semi-transparent and tandem photovoltaics.
{"title":"Active Selenium-Driven Confined Crystallization and Carrier Dynamics in High-Efficiency Ultrathin Semi-Transparent Sb2Se3 Solar Cells","authors":"Huafei Guo, Bangzhi Shen, Xing Wang, Jiayu Xiao, Wenyun Deng, Sai Jiang, Lei Xu, Xu Dong, LvZhou Li, Shuai Zhang, Jianhua Qiu, Ningyi Yuan, Jianning Ding","doi":"10.1039/d5sc08223d","DOIUrl":"https://doi.org/10.1039/d5sc08223d","url":null,"abstract":"To overcome the limited environmental stability of organic semi-transparent photovoltaic (STPV) devices, developing robust inorganic thin-film absorbers has become a critical research focus. Antimony selenide (Sb2Se3), with its Q1D crystal structure, excellent optoelectronic properties, and mechanical flexibility, is a promising candidate for STPV applications. However, thinning the absorber to enhance visible transmittance often degrades crystallinity, weakens preferred orientation, and increases defect density. Here, we present a dual-pathway device-engineering strategy that integrates KOH-assisted chemical-bath thinning of the CdS buffer layer with rapid thermal evaporation combined with magnetron sputtering of active selenium (Se). The introduced active Se atoms effectively reorganize molecular chains within a confined crystallization space, enhancing crystalline quality and promoting vertical [hk1] orientation. Simultaneously, Se doping passivates selenium vacancies and suppresses deep-level trap states, thereby improving carrier transport and reducing nonradiative recombination. Employing this strategy, we demonstrate for the first time an ultrathin Sb2Se3 STPV device with a total functional layer thickness of only 80 nm just one-seventh the thickness of conventional devices—achieving an efficiency of 7.02%, retaining 93% of that of thicker counterparts while maintaining an optical transparency exceeding 20%. This work establishes a practical route to simultaneously balance transparency and efficiency in inorganic STPV devices and underscores the potential of Sb2Se3 as a high-performance absorber for next-generation semi-transparent and tandem photovoltaics.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"82 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145947491","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}
Christian E Fajman, Dominik M Dankert, Peter Coburger, Wilhelm Klein, Thomas F Fässler
Intermetalloid clusters are considered as highly charged soluble models for intermetallic phases. While their bonding situation is not fully understood, their solubility makes them promising candidates for the fabrication of nanostructured intermetallic materials. We report on the synthesis of endohedral [TM@Tt9]4- (Tt = Sn and TM = Fe, Co, Ni, Pd; Tt = Pb and TM = Pd, Pt) clusters with Li counterions in solution. The potassium ions are replaced with lithium cations through a simple salt metathesis reaction using LiCl. The intermetalloid clusters crystallize in the known structure types known from compounds containing unfilled clusters. The new compounds are further investigated by Raman, NMR, and EPR spectroscopy.
{"title":"Endohedral Anionic Nine-Atom Zintl Clusters of the Elements Tin and Lead with Lithium Counterions","authors":"Christian E Fajman, Dominik M Dankert, Peter Coburger, Wilhelm Klein, Thomas F Fässler","doi":"10.1039/d5sc08011h","DOIUrl":"https://doi.org/10.1039/d5sc08011h","url":null,"abstract":"Intermetalloid clusters are considered as highly charged soluble models for intermetallic phases. While their bonding situation is not fully understood, their solubility makes them promising candidates for the fabrication of nanostructured intermetallic materials. We report on the synthesis of endohedral [TM@Tt9]4- (Tt = Sn and TM = Fe, Co, Ni, Pd; Tt = Pb and TM = Pd, Pt) clusters with Li counterions in solution. The potassium ions are replaced with lithium cations through a simple salt metathesis reaction using LiCl. The intermetalloid clusters crystallize in the known structure types known from compounds containing unfilled clusters. The new compounds are further investigated by Raman, NMR, and EPR spectroscopy.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"44 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145920465","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}
Donald G. Truhlar, Chengyi Zhang, Ruihu Lu, Qi Sun, Yu Mao, Tilo Söhnel, Yan Zhao, Ziyun Wang
Finding catalysts that have both high activity and high stability presents a long-standing challenge. Since optimizing activity and stability are conflicting objectives, the best one can do is find the Pareto front that yields optimal tradeoffs between these features. On the Pareto front, there is a trade-off where a portion of catalytic activity must be sacrificed to gain further stability and vice versa. Here, we provide a method to optimize the front by designing a multi-objective genetic algorithm that combines machine learning, graph neural network calculations, and density functional calculations. The application considered is the oxygen evolution reaction catalyzed by high-entropy alloys. We find that the Pareto front generally contains alloys with diverse elements, but that enhancing stability inevitably inflicts a toll on activity. We compare the general conclusions of our work to a survey of 545 experiments.
{"title":"Finding the Pareto front for high-entropy-alloy catalysts","authors":"Donald G. Truhlar, Chengyi Zhang, Ruihu Lu, Qi Sun, Yu Mao, Tilo Söhnel, Yan Zhao, Ziyun Wang","doi":"10.1039/d5sc06100h","DOIUrl":"https://doi.org/10.1039/d5sc06100h","url":null,"abstract":"Finding catalysts that have both high activity and high stability presents a long-standing challenge. Since optimizing activity and stability are conflicting objectives, the best one can do is find the Pareto front that yields optimal tradeoffs between these features. On the Pareto front, there is a trade-off where a portion of catalytic activity must be sacrificed to gain further stability and vice versa. Here, we provide a method to optimize the front by designing a multi-objective genetic algorithm that combines machine learning, graph neural network calculations, and density functional calculations. The application considered is the oxygen evolution reaction catalyzed by high-entropy alloys. We find that the Pareto front generally contains alloys with diverse elements, but that enhancing stability inevitably inflicts a toll on activity. We compare the general conclusions of our work to a survey of 545 experiments.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"254 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145947494","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}
Xinlei Ji, Keyi Zhou, My Ha Tran, Xi Chen, Ning Yan
Sustainable bioplastics have attracted considerable attention as alternatives to conventional petroleum-based plastics in response to growing concerns about resource depletion and environmental pollution. Natural biopolymers, such as starch, cellulose, and chitin/chitosan, are emerging as promising candidates for bioplastic production due to their widespread availability and biodegradability. This review conducts a comprehensive examination of recent advances in polymer-level structural engineering of natural biopolymers into bioplastics, with a focus on strategies that introduce intermolecular interactions, including permanent covalent bonds, dynamic covalent linkages, and noncovalent interactions, to reconstruct intrinsic hydrogen-bonded networks. This reconstruction provides the basis for converting natural biopolymers into bioplastics with permanent covalent, dynamic covalent, and physically crosslinked architectures, and the ways in which these architectures affect material properties, processability, and overall performance are systematically assessed. Additionally, the review discusses the direct utilization of raw lignocellulosic biomass as a potential approach to enhance the cost-effectiveness and scalability of bioplastic production. Finally, the challenges in developing high-performance bioplastics are examined, along with future perspectives for advancing bioplastics in alignment with circular economy principles and carbon neutrality objectives.
{"title":"Converting natural biopolymers to sustainable bioplastics via structure engineering","authors":"Xinlei Ji, Keyi Zhou, My Ha Tran, Xi Chen, Ning Yan","doi":"10.1039/d5sc07592k","DOIUrl":"https://doi.org/10.1039/d5sc07592k","url":null,"abstract":"Sustainable bioplastics have attracted considerable attention as alternatives to conventional petroleum-based plastics in response to growing concerns about resource depletion and environmental pollution. Natural biopolymers, such as starch, cellulose, and chitin/chitosan, are emerging as promising candidates for bioplastic production due to their widespread availability and biodegradability. This review conducts a comprehensive examination of recent advances in polymer-level structural engineering of natural biopolymers into bioplastics, with a focus on strategies that introduce intermolecular interactions, including permanent covalent bonds, dynamic covalent linkages, and noncovalent interactions, to reconstruct intrinsic hydrogen-bonded networks. This reconstruction provides the basis for converting natural biopolymers into bioplastics with permanent covalent, dynamic covalent, and physically crosslinked architectures, and the ways in which these architectures affect material properties, processability, and overall performance are systematically assessed. Additionally, the review discusses the direct utilization of raw lignocellulosic biomass as a potential approach to enhance the cost-effectiveness and scalability of bioplastic production. Finally, the challenges in developing high-performance bioplastics are examined, along with future perspectives for advancing bioplastics in alignment with circular economy principles and carbon neutrality objectives.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"9 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145947496","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}
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