Pub Date : 2024-11-13DOI: 10.1038/s41559-024-02582-7
Mohammad A. Siddiq, Fabien Duveau, Patricia J. Wittkopp
The environment influences how an organism’s genotype determines its phenotype and how this phenotype affects its fitness. Here, to better understand this dual role of environment in the production and selection of phenotypic variation, we determined genotype–phenotype–fitness relationships for mutant strains of Saccharomyces cerevisiae in four environments. Specifically, we measured how promoter mutations of the metabolic gene TDH3 modified expression level and affected growth for four different carbon sources. In each environment, we observed a clear relationship between TDH3 expression level and fitness, but this relationship differed among environments. Mutations with similar effects on expression in different environments often had different effects on fitness and vice versa. Such environment-specific relationships between phenotype and fitness can shape the evolution of phenotypic plasticity. We also found that mutations disrupting binding sites for transcription factors had more variable effects on expression among environments than those disrupting the TATA box, which is part of the core promoter. However, mutations with the most environmentally variable effects on fitness were located in the TATA box, because of both the lack of plasticity of TATA box mutations and environment-specific fitness functions. This observation suggests that mutations affecting different molecular mechanisms contribute unequally to regulatory sequence evolution in changing environments.
{"title":"Plasticity and environment-specific relationships between gene expression and fitness in Saccharomyces cerevisiae","authors":"Mohammad A. Siddiq, Fabien Duveau, Patricia J. Wittkopp","doi":"10.1038/s41559-024-02582-7","DOIUrl":"https://doi.org/10.1038/s41559-024-02582-7","url":null,"abstract":"<p>The environment influences how an organism’s genotype determines its phenotype and how this phenotype affects its fitness. Here, to better understand this dual role of environment in the production and selection of phenotypic variation, we determined genotype–phenotype–fitness relationships for mutant strains of <i>Saccharomyces cerevisiae</i> in four environments. Specifically, we measured how promoter mutations of the metabolic gene <i>TDH3</i> modified expression level and affected growth for four different carbon sources. In each environment, we observed a clear relationship between <i>TDH3</i> expression level and fitness, but this relationship differed among environments. Mutations with similar effects on expression in different environments often had different effects on fitness and vice versa. Such environment-specific relationships between phenotype and fitness can shape the evolution of phenotypic plasticity. We also found that mutations disrupting binding sites for transcription factors had more variable effects on expression among environments than those disrupting the TATA box, which is part of the core promoter. However, mutations with the most environmentally variable effects on fitness were located in the TATA box, because of both the lack of plasticity of TATA box mutations and environment-specific fitness functions. This observation suggests that mutations affecting different molecular mechanisms contribute unequally to regulatory sequence evolution in changing environments.</p>","PeriodicalId":13,"journal":{"name":"ACS Chemical Neuroscience","volume":"80 1","pages":""},"PeriodicalIF":16.8,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601079","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Electromethanation of CO2 has received intensive attention due to its high calorific value and convenient storage along with transportation to accommodate industrial demands. However, it is limited by sluggish multi-step proton-coupled electron transfer kinetics and undesired *H coupling under high current density, posing great challenges to its commercialization. Herein, carbon nitride (CN) with superior hydrogen adsorption ability is used as an active-hydrogen adsorption and supply material. Through a facile liquid-assisted exfoliation and electrostatic self-assembly strategy to strengthen its interfacial contacts with Cu2O catalysts, yielding a strengthened CH4 production 52 times higher than that of pristine Cu2O. Flow-cell test ultimately achieved FECH4 and remarkably CH4 partial current density of 61% and 561 mA cm−2, respectively. With in situ ATR-FTIR spectra and DFT calculations, it is established that strengthened interfaces enabled abundant *H tethered by ─C─N═C─ sites in CN nanosheets and oriented to the *CO hydrogenation to *CHO and *CHx on Cu species. This work reveals the profound influence of fine-expanded interfaces with dimensional materials on the product distribution and yield through the active-hydrogen management, which is of reference value for other small-molecule electro-polarization dominated by the proton-coupled electron transfer (PCET) process (e.g., N2, O2, etc.).
{"title":"Large-Current CO2 Electromethanation Through Active Hydrogen Regulation Over Carbon Nitride","authors":"Tianxiang Yan, Yaxin Jin, Qun Fan, Hai Liu, Xindi Li, Tianying Zhang, Hui Wang, Jianlong Lin, Haoyuan Chi, Sheng Zhang, Xinbin Ma","doi":"10.1002/smll.202408600","DOIUrl":"https://doi.org/10.1002/smll.202408600","url":null,"abstract":"Electromethanation of CO<sub>2</sub> has received intensive attention due to its high calorific value and convenient storage along with transportation to accommodate industrial demands. However, it is limited by sluggish multi-step proton-coupled electron transfer kinetics and undesired <sup>*</sup>H coupling under high current density, posing great challenges to its commercialization. Herein, carbon nitride (CN) with superior hydrogen adsorption ability is used as an active-hydrogen adsorption and supply material. Through a facile liquid-assisted exfoliation and electrostatic self-assembly strategy to strengthen its interfacial contacts with Cu<sub>2</sub>O catalysts, yielding a strengthened CH<sub>4</sub> production 52 times higher than that of pristine Cu<sub>2</sub>O. Flow-cell test ultimately achieved FE<sub>CH4</sub> and remarkably CH<sub>4</sub> partial current density of 61% and 561 mA cm<sup>−2</sup>, respectively. With in situ ATR-FTIR spectra and DFT calculations, it is established that strengthened interfaces enabled abundant <sup>*</sup>H tethered by ─C─N═C─ sites in CN nanosheets and oriented to the <sup>*</sup>CO hydrogenation to <sup>*</sup>CHO and <sup>*</sup>CHx on Cu species. This work reveals the profound influence of fine-expanded interfaces with dimensional materials on the product distribution and yield through the active-hydrogen management, which is of reference value for other small-molecule electro-polarization dominated by the proton-coupled electron transfer (PCET) process (e.g., N<sub>2</sub>, O<sub>2</sub>, etc.).","PeriodicalId":13,"journal":{"name":"ACS Chemical Neuroscience","volume":"69 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142610454","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Heavy atom effects can be used to enhance intermolecular interaction, regulate quinoidal resonance properties, increase bandwidths, and tune diradical characters, which have significant impacts on organic optoelectronic devices, such as organic field-effect transistors (OFETs), organic light-emitting diodes (OLEDs), organic photovoltaics (OPVs), etc. Meanwhile, the introduction of heavy atoms is shown to promote charge transfer, enhance air stability, and improve device performances in the field of organic thermoelectrics (OTEs). Thus, heavy atom effects are receiving more and more attention. However, regulating heavy atoms in organic semiconductors is still meeting great challenges. For example, heavy atoms will lead to solubility and stability issues (tellurium substitution) and lack of versatile design strategy and effective synthetic methods to be incorporated into organic semiconductors, which limit their application in electronic devices. Therefore, this work timely summarizes the unique functionalities of heavy atom effects, and up-to-date progress in organic electronics including OFETs, OPVs, OLEDs, and OTEs, while the structure-performance relationships between molecular designs and electronic devices are clearly elucidated. Furthermore, this review systematically analyzes the remaining challenges in regulating heavy atoms within organic semiconductors, and design strategies toward efficient and stable organic semiconductors by the introduction of novel heavy atoms regulation are proposed.
{"title":"Regulating Optoelectronic and Thermoelectric Properties of Organic Semiconductors by Heavy Atom Effects","authors":"Hao He, Ziting Zhong, Peng Fan, Wenchao Zhao, Dafei Yuan","doi":"10.1002/smll.202405156","DOIUrl":"https://doi.org/10.1002/smll.202405156","url":null,"abstract":"Heavy atom effects can be used to enhance intermolecular interaction, regulate quinoidal resonance properties, increase bandwidths, and tune diradical characters, which have significant impacts on organic optoelectronic devices, such as organic field-effect transistors (OFETs), organic light-emitting diodes (OLEDs), organic photovoltaics (OPVs), etc. Meanwhile, the introduction of heavy atoms is shown to promote charge transfer, enhance air stability, and improve device performances in the field of organic thermoelectrics (OTEs). Thus, heavy atom effects are receiving more and more attention. However, regulating heavy atoms in organic semiconductors is still meeting great challenges. For example, heavy atoms will lead to solubility and stability issues (tellurium substitution) and lack of versatile design strategy and effective synthetic methods to be incorporated into organic semiconductors, which limit their application in electronic devices. Therefore, this work timely summarizes the unique functionalities of heavy atom effects, and up-to-date progress in organic electronics including OFETs, OPVs, OLEDs, and OTEs, while the structure-performance relationships between molecular designs and electronic devices are clearly elucidated. Furthermore, this review systematically analyzes the remaining challenges in regulating heavy atoms within organic semiconductors, and design strategies toward efficient and stable organic semiconductors by the introduction of novel heavy atoms regulation are proposed.","PeriodicalId":13,"journal":{"name":"ACS Chemical Neuroscience","volume":"72 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601546","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yanwei Feng, Yongfeng Yuan, Gaoshen Cai, Bingxu Wang, Jun Zhang, Yang Xia, Shaoyi Guo
Interfacial pH fluctuation is one of the primary reasons for issues related to Zn metal anodes. Herein, polar amphoteric alanine, as a multifunctional electrolyte additive, is designed to regulate the electric double layer (EDL) and solvation structure. Alanine with self-adaptation capability to pH can stabilize electrolyte pH. Due to more negative adsorption energy, alanine preferentially adsorbs on the Zn surface and repels water molecules within the EDL. Alanine-enriched EDL effectively shields the surface tips, homogenizes interfacial electric field distribution, and promotes preferential deposition of horizontal flaky Zn. Alanine-enriched EDL limits the contact between water and the Zn anode. Alanine additive decreases the quantity of water molecules in the Zn2+ solvation sheath and disrupts H-bond networks in the electrolyte. Consequently, a dense and textured Zn deposition is achieved. Corrosion and side reactions are suppressed. Cycling stability of symmetrical cells attains 2700 h at 3 mA cm−2/1 mAh cm−2 and 2050 h at 5 mA cm−2/1 mAh cm−2. Average coulombic efficiency reaches 99.8% over 4500 cycles at 5 mA cm−2/1 mAh cm−2. Even within KOH alkaline electrolytes, alanine additive still improves the cycling lifespan of symmetrical cells to 100 h at 0.5 mA cm−2/0.5 mAh cm−2.
界面 pH 值波动是造成锌金属阳极相关问题的主要原因之一。在此，极性两性丙氨酸作为一种多功能电解质添加剂，旨在调节电双层（EDL）和溶解结构。具有 pH 自适应能力的丙氨酸可以稳定电解质的 pH 值。由于丙氨酸具有更高的负吸附能，它能优先吸附在 Zn 表面，并排斥 EDL 中的水分子。富含丙氨酸的 EDL 能有效屏蔽表面尖端，均匀界面电场分布，促进水平片状 Zn 的优先沉积。富含丙氨酸的 EDL 限制了水与锌阳极之间的接触。丙氨酸添加剂会减少 Zn2+ 溶剂鞘中的水分子数量，并破坏电解质中的氢键网络。因此，可以实现致密、纹理清晰的锌沉积。腐蚀和副反应受到抑制。对称电池在 3 mA cm-2/1 mAh cm-2 条件下的循环稳定性达到 2700 小时，在 5 mA cm-2/1 mAh cm-2 条件下达到 2050 小时。在 5 mA cm-2/1 mAh cm-2 条件下循环 4500 次，平均库仑效率达到 99.8%。即使在 KOH 碱性电解质中，丙氨酸添加剂仍可将对称电池的循环寿命提高到 100 小时（0.5 mA cm-2/0.5 mAh cm-2）。
{"title":"Multifunctional Amphoteric Additive Alanine Enables High-Performance Wide-pH Zn Metal Anodes","authors":"Yanwei Feng, Yongfeng Yuan, Gaoshen Cai, Bingxu Wang, Jun Zhang, Yang Xia, Shaoyi Guo","doi":"10.1002/smll.202405144","DOIUrl":"https://doi.org/10.1002/smll.202405144","url":null,"abstract":"Interfacial pH fluctuation is one of the primary reasons for issues related to Zn metal anodes. Herein, polar amphoteric alanine, as a multifunctional electrolyte additive, is designed to regulate the electric double layer (EDL) and solvation structure. Alanine with self-adaptation capability to pH can stabilize electrolyte pH. Due to more negative adsorption energy, alanine preferentially adsorbs on the Zn surface and repels water molecules within the EDL. Alanine-enriched EDL effectively shields the surface tips, homogenizes interfacial electric field distribution, and promotes preferential deposition of horizontal flaky Zn. Alanine-enriched EDL limits the contact between water and the Zn anode. Alanine additive decreases the quantity of water molecules in the Zn<sup>2+</sup> solvation sheath and disrupts H-bond networks in the electrolyte. Consequently, a dense and textured Zn deposition is achieved. Corrosion and side reactions are suppressed. Cycling stability of symmetrical cells attains 2700 h at 3 mA cm<sup>−2</sup>/1 mAh cm<sup>−2</sup> and 2050 h at 5 mA cm<sup>−2</sup>/1 mAh cm<sup>−2</sup>. Average coulombic efficiency reaches 99.8% over 4500 cycles at 5 mA cm<sup>−2</sup>/1 mAh cm<sup>−2</sup>. Even within KOH alkaline electrolytes, alanine additive still improves the cycling lifespan of symmetrical cells to 100 h at 0.5 mA cm<sup>−2</sup>/0.5 mAh cm<sup>−2</sup>.","PeriodicalId":13,"journal":{"name":"ACS Chemical Neuroscience","volume":"65 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601549","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-13DOI: 10.1016/j.cej.2024.157656
Junpeng Jiang, Liwen Yan, Jiangtao Li, Yunjia Xue, Chensi Zhang, Xiaoxia Hu, Anran Guo, Haiyan Du, Jiachen Liu
Owing to tunable dielectric properties, light weight and high porosity, polymer-derived SiBCN ceramic aerogels possess significant application prospects in electromagnetic wave (EMW) absorption and thermal insulation. However, due to inadequate oxidation resistance, the structural collapse and performance deterioration of SiBCN aerogels will easily occur in high-temperature aerobic environments, limiting their application. Herein, to address this issue, a novel and straightforward strategy based on typical polymer-derived-ceramic (PDC) aerogel method and impregnation with boehmite sol was proposed for synthesizing SiBCN/Al2O3 composite ceramic aerogels. The microstructure, phase composition, thermal insulation, oxidation resistance and EMW absorption properties of SiBCN/Al2O3 ceramic aerogels were investigated. The resulting SiBCN/Al2O3 composite aerogel demonstrates superior high-temperature structural stability, exhibiting an ultra-low linear shrinkage of only 6.5 % following heat treatment at 1200 °C for 2 h in air. Additionally, the composite aerogel shows a low thermal conductivity of 0.039 W/mK and a low density of 0.112 g/cm3. The SiBCN/Al2O3 composite aerogel, composed of dielectric SiBCN, conductive free carbon, and insulating alumina, demonstrates outstanding EMW absorption properties with a minimum reflection loss of −48.6 dB and an effective bandwidth of 5.8 GHz. The enhanced microwave absorption performance is mainly attributed to the improved impedance matching, multiple reflection, and enhanced interfacial polarization resulting from the introduction of Al2O3. Given prominent oxidation resistance, thermal insulation and EMW absorption properties, the SiBCN/Al2O3 composite aerogel paves the way for developing microwave absorption and thermal insulation integrated material in high-speed vehicles.
{"title":"Lightweight, thermally insulating SiBCN/Al2O3 ceramic aerogel with enhanced high-temperature resistance and electromagnetic wave absorption performance","authors":"Junpeng Jiang, Liwen Yan, Jiangtao Li, Yunjia Xue, Chensi Zhang, Xiaoxia Hu, Anran Guo, Haiyan Du, Jiachen Liu","doi":"10.1016/j.cej.2024.157656","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157656","url":null,"abstract":"Owing to tunable dielectric properties, light weight and high porosity, polymer-derived SiBCN ceramic aerogels possess significant application prospects in electromagnetic wave (EMW) absorption and thermal insulation. However, due to inadequate oxidation resistance, the structural collapse and performance deterioration of SiBCN aerogels will easily occur in high-temperature aerobic environments, limiting their application. Herein, to address this issue, a novel and straightforward strategy based on typical polymer-derived-ceramic (PDC) aerogel method and impregnation with boehmite sol was proposed for synthesizing SiBCN/Al<sub>2</sub>O<sub>3</sub> composite ceramic aerogels. The microstructure, phase composition, thermal insulation, oxidation resistance and EMW absorption properties of SiBCN/Al<sub>2</sub>O<sub>3</sub> ceramic aerogels were investigated. The resulting SiBCN/Al<sub>2</sub>O<sub>3</sub> composite aerogel demonstrates superior high-temperature structural stability, exhibiting an ultra-low linear shrinkage of only 6.5 % following heat treatment at 1200 °C for 2 h in air. Additionally, the composite aerogel shows a low thermal conductivity of 0.039 W/mK and a low density of 0.112 g/cm<sup>3</sup>. The SiBCN/Al<sub>2</sub>O<sub>3</sub> composite aerogel, composed of dielectric SiBCN, conductive free carbon, and insulating alumina, demonstrates outstanding EMW absorption properties with a minimum reflection loss of −48.6 dB and an effective bandwidth of 5.8 GHz. The enhanced microwave absorption performance is mainly attributed to the improved impedance matching, multiple reflection, and enhanced interfacial polarization resulting from the introduction of Al<sub>2</sub>O<sub>3</sub>. Given prominent oxidation resistance, thermal insulation and EMW absorption properties, the SiBCN/Al<sub>2</sub>O<sub>3</sub> composite aerogel paves the way for developing microwave absorption and thermal insulation integrated material in high-speed vehicles.","PeriodicalId":13,"journal":{"name":"ACS Chemical Neuroscience","volume":"157 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601370","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Qinhui Bao, Chuwu Xing, Miao He, Zhiwei Nie, Rihua Wang, Chunsheng Wan, Tianjin Zhang, Duofa Wang
The subsurface of perovskite (PVK) triggers non-radiative recombination and initiates film degradation due to the impurities and defects. This study investigates the limitations of the conventional surface post-treatment and proposes an innovative pre-treatment strategy to achieve complete impurity elimination and defect passivation of the subsurface. The considerable activity of unannealed PVK films provides a sufficient basis for effective subsurface modification. Following the pre-treatment, the cadmium ions (Cd2+) can occupy the lead (Pb) vacancies or substitute lead ions(Pb2+), while the introduced ionic ions (I-) are able to fill the ionic (I) vacancies. The stronger ionic bond between Cd2+ and I− helps prevent the loss of I-, leading to a reduction of defects in film, inhibiting non-radiative recombination and ionic migration at the interface. This innovative strategy successfully eliminates impurities and passivates defects, resulting in a perovskite subsurface characterized by high crystallinity, low defect density, and minimal impurity. These enhancements contribute to enhanced open circuit voltage (VOC)and fill factor (FF), leading to an impressive power conversion efficiency (PCE) of 24.49%. Notably, after 1600 h of aging in ambient air, the cell retained 87% of its initial performance.
{"title":"High-Quality Subsurface Construction of Perovskite Film for Efficient and Stable Solar Cells","authors":"Qinhui Bao, Chuwu Xing, Miao He, Zhiwei Nie, Rihua Wang, Chunsheng Wan, Tianjin Zhang, Duofa Wang","doi":"10.1002/smll.202406386","DOIUrl":"https://doi.org/10.1002/smll.202406386","url":null,"abstract":"The subsurface of perovskite (PVK) triggers non-radiative recombination and initiates film degradation due to the impurities and defects. This study investigates the limitations of the conventional surface post-treatment and proposes an innovative pre-treatment strategy to achieve complete impurity elimination and defect passivation of the subsurface. The considerable activity of unannealed PVK films provides a sufficient basis for effective subsurface modification. Following the pre-treatment, the cadmium ions (Cd<sup>2+</sup>) can occupy the lead (Pb) vacancies or substitute lead ions(Pb<sup>2+</sup>), while the introduced ionic ions (I<sup>-</sup>) are able to fill the ionic (I) vacancies. The stronger ionic bond between Cd<sup>2+</sup> and I<sup>−</sup> helps prevent the loss of I<sup>-</sup>, leading to a reduction of defects in film, inhibiting non-radiative recombination and ionic migration at the interface. This innovative strategy successfully eliminates impurities and passivates defects, resulting in a perovskite subsurface characterized by high crystallinity, low defect density, and minimal impurity. These enhancements contribute to enhanced open circuit voltage (V<sub>OC</sub>)and fill factor (FF), leading to an impressive power conversion efficiency (PCE) of 24.49%. Notably, after 1600 h of aging in ambient air, the cell retained 87% of its initial performance.","PeriodicalId":13,"journal":{"name":"ACS Chemical Neuroscience","volume":"17 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142610452","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Carrier selective contacts with passivation effects are considered to have a significant influence on the performance of crystalline silicon (c-Si) solar cells. It is essential for electron selective contact materials to meet the requirements of ultra-low contact resistance and excellent passivation effects. This work introduces a stack layer of Lithium Phosphate (Li3PO4) /Titanium Dioxide (TiO2) as a new electron selective passivating contact. It is found that the stack achieves an impressive contact resistivity (ρc) of 0.128 mΩ cm2 on n-type c-Si substrates with resistivity ranging from 1 to 3 Ω cm (14.6 mΩ cm2 for the n-Si/a-Si:H/Li3PO4/TiO2/Al contact). Furthermore, it effectively reduces the surface recombination parameter (J0) to less than 4 fA by incorporating a 6 nm a-Si:H(i) layer. The characterization of the n-Si/Li3PO4/TiO2 interface reveals that phosphorus diffusion into silicon plays a crucial role in achieving the ultra-low contact resistivity, while the presence of PO43− groups helps in fixing hydrogen atoms to maintain the desired chemical passivation effect. Finally, a silicon heterojunction solar cell (SHJ) with a rear full-area configuration of a-Si:H/Li3PO4/TiO2/Al is successfully demonstrated achieving an impressive power conversion efficiency of 22.89%. The result proves the efficacy of employing hydrogen-rich low-work function metal oxide stacks as electron selective passivating contacts.
{"title":"Self-Diffusion Effect Assisted TiO2/Li3PO4 Electron Selective Passivating Contact in Silicon Solar Cells Approaching 23% Efficiency","authors":"Zhiyuan Xu, Yu Yan, Wei Li, Qianfeng Gao, Yaya Song, Maobin Zhang, Junming Xue, Huizhi Ren, Shengzhi Xu, Xinliang Chen, Yi Ding, Qian Huang, Xiaodan Zhang, Ying Zhao, Guofu Hou","doi":"10.1002/smll.202407398","DOIUrl":"https://doi.org/10.1002/smll.202407398","url":null,"abstract":"Carrier selective contacts with passivation effects are considered to have a significant influence on the performance of crystalline silicon (c-Si) solar cells. It is essential for electron selective contact materials to meet the requirements of ultra-low contact resistance and excellent passivation effects. This work introduces a stack layer of Lithium Phosphate (Li<sub>3</sub>PO<sub>4</sub>) /Titanium Dioxide (TiO<sub>2</sub>) as a new electron selective passivating contact. It is found that the stack achieves an impressive contact resistivity (<i>ρ</i><sub>c</sub>) of 0.128 mΩ cm<sup>2</sup> on n-type c-Si substrates with resistivity ranging from 1 to 3 Ω cm (14.6 mΩ cm<sup>2</sup> for the n-Si/a-Si:H/Li<sub>3</sub>PO<sub>4</sub>/TiO<sub>2</sub>/Al contact). Furthermore, it effectively reduces the surface recombination parameter (<i>J</i><sub>0</sub>) to less than 4 fA by incorporating a 6 nm a-Si:H(i) layer. The characterization of the n-Si/Li<sub>3</sub>PO<sub>4</sub>/TiO<sub>2</sub> interface reveals that phosphorus diffusion into silicon plays a crucial role in achieving the ultra-low contact resistivity, while the presence of PO<sub>4</sub><sup>3−</sup> groups helps in fixing hydrogen atoms to maintain the desired chemical passivation effect. Finally, a silicon heterojunction solar cell (SHJ) with a rear full-area configuration of a-Si:H/Li<sub>3</sub>PO<sub>4</sub>/TiO<sub>2</sub>/Al is successfully demonstrated achieving an impressive power conversion efficiency of 22.89%. The result proves the efficacy of employing hydrogen-rich low-work function metal oxide stacks as electron selective passivating contacts.","PeriodicalId":13,"journal":{"name":"ACS Chemical Neuroscience","volume":"13 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142610453","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-13DOI: 10.1021/acschemneuro.4c00369
A N Resmi, Shaiju S Nazeer, M E Dhushyandhun, Willi Paul, Binu P Chacko, Ramshekhar N Menon, Ramapurath S Jayasree
Accurate and early disease detection is crucial for improving patient care, but traditional diagnostic methods often fail to identify diseases in their early stages, leading to delayed treatment outcomes. Early diagnosis using blood derivatives as a source for biomarkers is particularly important for managing Alzheimer's disease (AD). This study introduces a novel approach for the precise and ultrasensitive detection of multiple core AD biomarkers (Aβ40, Aβ42, p-tau, and t-tau) using surface-enhanced Raman spectroscopy (SERS) combined with machine-learning algorithms. Our method employs an antibody-immobilized aluminum SERS substrate, which offers high precision, sensitivity, and accuracy. The platform achieves an impressive detection limit in the attomolar (aM) range and spans a wide dynamic range from aM to micromolar (μM) concentrations. This ultrasensitive and specific SERS immunoassay platform shows promise for identifying mild cognitive impairment (MCI), a potential precursor to AD, from blood plasma. Machine-learning algorithms applied to the spectral data enhance the differentiation of MCI from AD and healthy controls, yielding excellent sensitivity and specificity. Our integrated SERS-machine-learning approach, with its interpretability, advances AD research and underscores the effectiveness of a cost-efficient, easy-to-prepare Al-SERS substrate for clinical AD detection.
{"title":"Ultrasensitive Detection of Blood-Based Alzheimer's Disease Biomarkers: A Comprehensive SERS-Immunoassay Platform Enhanced by Machine Learning.","authors":"A N Resmi, Shaiju S Nazeer, M E Dhushyandhun, Willi Paul, Binu P Chacko, Ramshekhar N Menon, Ramapurath S Jayasree","doi":"10.1021/acschemneuro.4c00369","DOIUrl":"https://doi.org/10.1021/acschemneuro.4c00369","url":null,"abstract":"<p><p>Accurate and early disease detection is crucial for improving patient care, but traditional diagnostic methods often fail to identify diseases in their early stages, leading to delayed treatment outcomes. Early diagnosis using blood derivatives as a source for biomarkers is particularly important for managing Alzheimer's disease (AD). This study introduces a novel approach for the precise and ultrasensitive detection of multiple core AD biomarkers (Aβ<sub>40</sub>, Aβ<sub>42</sub>, p-tau, and t-tau) using surface-enhanced Raman spectroscopy (SERS) combined with machine-learning algorithms. Our method employs an antibody-immobilized aluminum SERS substrate, which offers high precision, sensitivity, and accuracy. The platform achieves an impressive detection limit in the attomolar (aM) range and spans a wide dynamic range from aM to micromolar (μM) concentrations. This ultrasensitive and specific SERS immunoassay platform shows promise for identifying mild cognitive impairment (MCI), a potential precursor to AD, from blood plasma. Machine-learning algorithms applied to the spectral data enhance the differentiation of MCI from AD and healthy controls, yielding excellent sensitivity and specificity. Our integrated SERS-machine-learning approach, with its interpretability, advances AD research and underscores the effectiveness of a cost-efficient, easy-to-prepare Al-SERS substrate for clinical AD detection.</p>","PeriodicalId":13,"journal":{"name":"ACS Chemical Neuroscience","volume":" ","pages":""},"PeriodicalIF":4.1,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142612709","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The development of near-infrared (NIR) luminescent materials featuring high photoluminescence quantum yield (ΦPL) at aggregated state is of great significance for achieving highly efficient non-doped organic light-emitting diodes (OLEDs) but remains formidable challenging. Herein, a design strategy of introducing electron-rich thiophene groups between electron acceptor and donor is proposed for efficient NIR luminescent materials, and a tailored D-π-A-π-D type emitter, namely, 4,4′-(benzo[c][1], [2], [5]thiadiazole-4,7-diylbis(thiophene-5,2-diyl))bis(N,N-diphenylaniline) (TPATBT), is designed and prepared. The photophysical investigation and density functional theory analysis disclose that TPATBT is a hot exciton emitter feature with hybridized local and charge-transfer state. Additionally, TPATBT demonstrates aggregation-induced emission characteristic, prefers high thermal stability, and exhibits a strong emission at 692 nm with a decent ΦPL of 20 % in the neat film. The non-doped device based on TPATBT neat film presents a maximum external quantum efficiency (ηext,max) of 1.22 % with electroluminescence peak at 718n m. Moreover, we first try to use interlayer sensitization to sensitize non-doped devices, which achieves better ηext,max of 1.34 % with low turn-on voltage of 3.2 V. The proposed molecular design strategy in this work is promising for exploring robust NIR luminescent materials for high-performance OLEDs.
{"title":"Introducing electron-rich thiophene bridges in hot exciton emitter for efficient non-Doped near-infrared OLEDs with low turn-on voltages","authors":"Ruming Jiang, Zhangshan Liu, Yuanyuan Han, Jiawei Long, Ting Guo, Xia Lan, Mingguang Yu, Ting Fan, Haijun Ma, Yen Wei, Ben Zhong Tang, Zujin Zhao","doi":"10.1016/j.cej.2024.157575","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157575","url":null,"abstract":"The development of near-infrared (NIR) luminescent materials featuring high photoluminescence quantum yield (Φ<sub>PL</sub>) at aggregated state is of great significance for achieving highly efficient non-doped organic light-emitting diodes (OLEDs) but remains formidable challenging. Herein, a design strategy of introducing electron-rich thiophene groups between electron acceptor and donor is proposed for efficient NIR luminescent materials, and a tailored D-π-A-π-D type emitter, namely, 4,4′-(benzo[c]<span><span>[1]</span></span>, <span><span>[2]</span></span>, <span><span>[5]</span></span>thiadiazole-4,7-diylbis(thiophene-5,2-diyl))bis(N,N-diphenylaniline) (TPATBT), is designed and prepared. The photophysical investigation and density functional theory analysis disclose that TPATBT is a hot exciton emitter feature with hybridized local and charge-transfer state. Additionally, TPATBT demonstrates aggregation-induced emission characteristic, prefers high thermal stability, and exhibits a strong emission at 692 nm with a decent Φ<sub>PL</sub> of 20 % in the neat film. The non-doped device based on TPATBT neat film presents a maximum external quantum efficiency (η<sub>ext,max</sub>) of 1.22 % with electroluminescence peak at 718n m. Moreover, we first try to use interlayer sensitization to sensitize non-doped devices, which achieves better η<sub>ext,max</sub> of 1.34 % with low turn-on voltage of 3.2 V. The proposed molecular design strategy in this work is promising for exploring robust NIR luminescent materials for high-performance OLEDs.","PeriodicalId":13,"journal":{"name":"ACS Chemical Neuroscience","volume":"10 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142599552","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Tong Wu, Xueqian Zhang, Quan Xu, Lehui Wang, Yao Li, Xiaohan Jiang, Qingwei Wang, Weili Zhang, Jiaguang Han
The ability to achieve independent complex amplitude control across multiple channels can significantly increase the information capacity of photonic devices. Diffraction inherently holds numerous channels, which are good candidates for dense light manipulation in angular space. However, no convenient method is currently available for attaining this. Here, a flexible interference approach utilizing silicon-based transmission-type heterogeneous-gradient supercell metasurfaces is proposed. By simply designing the phases of the meta-atoms’ radiations within a supercell, the complex amplitude of each diffraction channel can be individually and analytically controlled. Crucially, the complex amplitudes of multiple diffraction channels can be simultaneously controlled in a non-interleaved manner, where the number of channels is determined by the number of effective adjusting degrees of freedom (DoF). As a proof-of-concept validation, several meta-devices are experimentally demonstrated in the terahertz regime, which can generate multiple vortex beams, focal points, and splitting beams in different desired diffraction angles. This advancement heralds a new pathway for the development of multifunctional photonic devices with enhanced channel capacity, offering significant potential for both research and practical applications in photonics.
{"title":"Heterogeneous-Gradient Supercell Metasurfaces for Independent Complex Amplitude Control over Multiple Diffraction Channels","authors":"Tong Wu, Xueqian Zhang, Quan Xu, Lehui Wang, Yao Li, Xiaohan Jiang, Qingwei Wang, Weili Zhang, Jiaguang Han","doi":"10.1002/smll.202407303","DOIUrl":"https://doi.org/10.1002/smll.202407303","url":null,"abstract":"The ability to achieve independent complex amplitude control across multiple channels can significantly increase the information capacity of photonic devices. Diffraction inherently holds numerous channels, which are good candidates for dense light manipulation in angular space. However, no convenient method is currently available for attaining this. Here, a flexible interference approach utilizing silicon-based transmission-type heterogeneous-gradient supercell metasurfaces is proposed. By simply designing the phases of the meta-atoms’ radiations within a supercell, the complex amplitude of each diffraction channel can be individually and analytically controlled. Crucially, the complex amplitudes of multiple diffraction channels can be simultaneously controlled in a non-interleaved manner, where the number of channels is determined by the number of effective adjusting degrees of freedom (DoF). As a proof-of-concept validation, several meta-devices are experimentally demonstrated in the terahertz regime, which can generate multiple vortex beams, focal points, and splitting beams in different desired diffraction angles. This advancement heralds a new pathway for the development of multifunctional photonic devices with enhanced channel capacity, offering significant potential for both research and practical applications in photonics.","PeriodicalId":13,"journal":{"name":"ACS Chemical Neuroscience","volume":"4 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142599938","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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