ACS Publications最新文献_第3页

Unambiguous Detection of LTR-III G-Quadruplex in the HIV Genome Using a Tailored Fluorogenic Probe-based Assay. 使用基于定制荧光探针的检测方法明确检测 HIV 基因组中的 LTR-III G-四重链。

IF 6.7 1区化学

Analytical Chemistry Pub Date : 2024-09-24 DOI: 10.1021/acs.analchem.4c03374

Sumon Pratihar, Vasudhar Bhat S V, Krithi K Bhagavath, Thimmaiah Govindaraju

引用次数: 0

Enzyme Tunnel Dynamics and Catalytic Mechanism of Norcoclaurine Synthase: Insights from a Combined LiGaMD and DFT Study. 去甲古柯碱合成酶的酶隧道动力学和催化机理：LiGaMD 和 DFT 联合研究的启示。

IF 2.8 2区化学

The Journal of Physical Chemistry B Pub Date : 2024-09-24 DOI: 10.1021/acs.jpcb.4c04243

Xujian Wang, Haodong Liu, Jingyao Wang, Le Chang, Jiayang Cai, Zexuan Wei, Jiayu Pan, Xiaohui Gu, Wan-Lu Li, Jiahuang Li

{"title":"Enzyme Tunnel Dynamics and Catalytic Mechanism of Norcoclaurine Synthase: Insights from a Combined LiGaMD and DFT Study.","authors":"Xujian Wang, Haodong Liu, Jingyao Wang, Le Chang, Jiayang Cai, Zexuan Wei, Jiayu Pan, Xiaohui Gu, Wan-Lu Li, Jiahuang Li","doi":"10.1021/acs.jpcb.4c04243","DOIUrl":"https://doi.org/10.1021/acs.jpcb.4c04243","url":null,"abstract":"This study conducts a systematic investigation into the catalytic mechanism of norcoclaurine synthase (NCS), a key enzyme in the biosynthesis of tetrahydroisoquinolines (THIQs) with therapeutic applications. By integration of LiGaMD and DFT calculations, the reaction pathway of NCS is mapped, providing detailed insights into its catalytic activity and selectivity. Our findings underscore the critical role of E103 in substrate capture and reveal the hitherto unappreciated influence of nonpolar residues M183 and L76 on tunnel dynamics. A prominent discovery is the identification of a high-energy barrier (44.2 kcal/mol) associated with the aromatic electrophilic attack, which pinpoints the rate-limiting step. Moreover, we disclose the existence of dual transition states leading to different products with the energetically favored six-membered ring formation consistent with experimental evidence. These mechanistic revelations not only refine our understanding of NCS but also advocate for a renewed emphasis on enzyme tunnel engineering for optimizing THIQs biosynthesis. The research sets the stage for translating these findings into practical enzyme modifications. Our results highlight the potential of NCS as a biocatalyst to overcome the limitations of current synthetic methodologies, such as low yields and environmental impacts, and provide a theoretical contribution to the efficient, eco-friendly production of THIQs-based pharmaceuticals.","PeriodicalId":60,"journal":{"name":"The Journal of Physical Chemistry B","volume":null,"pages":null},"PeriodicalIF":2.8,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142306639","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Catalytic Asymmetric Hydrogen Atom Transfer Based on a Chiral Hydrogen Atom Donor Generated from TBADT and Chiral BINOL. 基于 TBADT 和手性 BINOL 生成的手性氢原子供体的催化不对称氢原子转移。

IF 4.9 1区化学

Organic Letters Pub Date : 2024-09-24 DOI: 10.1021/acs.orglett.4c03175

Ling Li, Shi-Qi Zhang, Xin Cui, Gang Zhao, Zhuo Tang, Guang-Xun Li

引用次数: 0

An Ultrasensitive Bi₂O₂Se/In₂S₃ Photodetector with Low Detection Limit and Fast Response toward High-Precision Unmanned Driving. 一种超灵敏的 Bi2O2Se/In2S3 光电探测器，检测限低、响应快，可用于高精度无人驾驶。

IF 15.8 1区材料科学

ACS Nano Pub Date : 2024-09-24 DOI: 10.1021/acsnano.4c08636

Meifei Chen, Xiqiang Chen, Ziqiao Wu, Zihao Huang, Wei Gao, Mengmeng Yang, Ye Xiao, Yu Zhao, Zhaoqiang Zheng, Jiandong Yao, Jingbo Li

{"title":"An Ultrasensitive Bi2O2Se/In2S3 Photodetector with Low Detection Limit and Fast Response toward High-Precision Unmanned Driving.","authors":"Meifei Chen, Xiqiang Chen, Ziqiao Wu, Zihao Huang, Wei Gao, Mengmeng Yang, Ye Xiao, Yu Zhao, Zhaoqiang Zheng, Jiandong Yao, Jingbo Li","doi":"10.1021/acsnano.4c08636","DOIUrl":"https://doi.org/10.1021/acsnano.4c08636","url":null,"abstract":"The machine vision utilized in unmanned driving systems must possess the ability to accurately perceive scenes under low-light illumination conditions. To achieve this, photodetectors with low detection limits and a fast response are essential. Current systems rely on avalanche diodes or lidars, which come with the drawbacks of increased energy consumption and complexity. Here, we present an ultrasensitive photodetector based on a two-dimensional (2D) Bi2O2Se/In2S3 heterostructure, incorporating a homotype unilateral depletion band design. This innovative architecture effectively modulates the transport of both free and photoexcited carriers, suppressing the dark current and facilitating the rapid and efficient separation of photocarriers. Owing to these features, this device exhibits a responsivity of 144 A/W, a specific detectivity of 1.2 × 1014 Jones, and a light on/off ratio of 1.1 × 105. These metrics rank among the top values reported for state-of-the-art 2D devices. Moreover, this device also demonstrates a fast response time of 170/296 μs and a low noise equivalent power of 0.57 fW/Hz1/2, attributes that endow it with ultraweak light imaging capabilities. Furthermore, we have successfully integrated this device into an unmanned driving system, providing a perspective on the design and fabrication of future optoelectronic devices.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":null,"pages":null},"PeriodicalIF":15.8,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142306526","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

A DNA Molecular Logic Circuit for Precise Tumor Identification. 精确识别肿瘤的 DNA 分子逻辑电路

IF 9.6 1区材料科学

Nano Letters Pub Date : 2024-09-24 DOI: 10.1021/acs.nanolett.4c02342

Yingyu Sima, Lili Ai, Linlin Wang, Pengge Zhang, Qiang Zhang, Shanchao Wu, Sitao Xie, Zilong Zhao, Weihong Tan

引用次数: 0

Pickering Emulsion Promoted Interfacial Sequential Chemo-Biocatalytic Reaction for the Synthesis of Chiral Alcohols from Styrene. 以苯乙烯为原料合成手性醇的 Pickering Emulsion Promoted Interfacial Sequential Chemo-Biocatalytic Reaction。

IF 8.3 2区材料科学

ACS Applied Materials & Interfaces Pub Date : 2024-09-24 DOI: 10.1021/acsami.4c10461

Weiqi Wang, Yuting Yu, Mengyao Wang, Yangxin Wang, Shanqiu Liu, Jian Xu, Zhiyong Sun

{"title":"Pickering Emulsion Promoted Interfacial Sequential Chemo-Biocatalytic Reaction for the Synthesis of Chiral Alcohols from Styrene.","authors":"Weiqi Wang, Yuting Yu, Mengyao Wang, Yangxin Wang, Shanqiu Liu, Jian Xu, Zhiyong Sun","doi":"10.1021/acsami.4c10461","DOIUrl":"https://doi.org/10.1021/acsami.4c10461","url":null,"abstract":"Chemo-biocatalytic cascades have emerged as a promising approach in the realm of advanced synthesis. However, reconciling the incompatible reaction conditions among distinct catalytic species presents a significant challenge. Herein, we introduce an innovative solution using an emulsion system stabilized by Janus silica nanoparticles, which serve as a bridge for both chemo-catalysts and biocatalysts at the interface. The chemo-catalyst is securely anchored within a hydrophobic polymer matrix, ensuring its residence in an organic environment. Meanwhile, the negatively charged E. coli cells containing enzymes are attracted to the aqueous phase at the interface, facilitating their optimal positioning. We demonstrate the efficacy of this system through a two-step cascade reaction. Initially, the oxidation of styrene to acetophenone using palladium as a chemocatalyst achieves a 6-fold increase in yield compared to the control system. Subsequently, the reduction of achiral acetophenone to its chiral alcohol derivative presents a 17-fold yield enhancement relative to that of the control reaction. Importantly, our system exhibits versatility, accommodating a wide range of substrates for both individual and sequential reactions. This work not only validates the concept but also paves the way for the integration of chemo- and biocatalysts in the synthesis of a broader array of high-value chemical compounds.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":null,"pages":null},"PeriodicalIF":8.3,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142306545","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Induced Extracellular Ice Nucleation Protects Cocultured Spheroid Interior and Exterior during Cryopreservation. 诱导细胞外冰核在冷冻保存过程中保护球形细胞的内部和外部

IF 5.4 2区医学

ACS Biomaterials Science & Engineering Pub Date : 2024-09-24 DOI: 10.1021/acsbiomaterials.4c00958

Yanan Gao, Akalabya Bissoyi, Qiongyu Guo, Matthew I Gibson

引用次数: 0

The Next Twenty Years of the Journal of Chemical Theory and Computation 化学理论与计算》杂志的下一个二十年

IF 5.7 1区化学

Journal of Chemical Theory and Computation Pub Date : 2024-09-24 DOI: 10.1021/acs.jctc.4c0106710.1021/acs.jctc.4c01067

Qiang Cui, Marco De Vivo and Laura Gagliardi*,

引用次数: 0

Foldable Metamaterial Absorber with Liquid Metal Printing on Paper. 纸上印刷液态金属的可折叠超材料吸收器

IF 8.3 2区材料科学

ACS Applied Materials & Interfaces Pub Date : 2024-09-24 DOI: 10.1021/acsami.4c12021

Jinwoo Ho, Woochan Kim, Daeyoung Kim, Sang Kug Chung, Sungjoon Lim

{"title":"Foldable Metamaterial Absorber with Liquid Metal Printing on Paper.","authors":"Jinwoo Ho, Woochan Kim, Daeyoung Kim, Sang Kug Chung, Sungjoon Lim","doi":"10.1021/acsami.4c12021","DOIUrl":"https://doi.org/10.1021/acsami.4c12021","url":null,"abstract":"Metamaterials, characterized by their unique artificial periodic structures, exhibit extraordinary abilities in controlling electromagnetic waves not found in natural materials. Metamaterial absorbers, for example, have been developed by patterning solid conductive materials on dielectric surfaces. However, the foldability limitations of solid conductors make them unsuitable as foldable metamaterial absorbers since they lose those desirable properties when folded. To address this challenge, various methods using liquid metals have emerged, but they either require often necessitate structural frames or are primarily suited for hard surfaces, limiting their foldability potential. This study proposes an innovative solution involving the deposition of liquid metal onto paper surfaces to overcome foldability constraints. We design a metamaterial absorber with a circular pattern using three sheets of printing paper bonded with a film, leveraging these adhesive properties of oxidized gallium-based liquid metal to waterproof agent coated printing paper while preventing adhesion to laser-printed toner surfaces. The experimental results show that this absorber achieves an absorption rate of more than 90% in the frequency range of 10.36-10.76 GHz while being insensitive to polarization and incidence angle. Surprisingly, our proposed absorber retains its excellent performance even after being folded and unfolded up to 50 times. This foldable metamaterial absorber made of liquid metal is a promising solution for electromagnetic wave management applications requiring flexibility and adaptability.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":null,"pages":null},"PeriodicalIF":8.3,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142306523","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Toughness and Thermoresponsive Hydrogel for Sandwich Smart Window with Adaptive Solar Modulation and Energy Saving. 用于具有自适应太阳能调节和节能功能的夹层智能窗的韧性和热致伸缩性水凝胶

IF 8.3 2区材料科学

ACS Applied Materials & Interfaces Pub Date : 2024-09-24 DOI: 10.1021/acsami.4c13133

Huijie Guan, Yinghan Lu, Yijiang You, Shengxiang Gao, Li Liu, Guangfeng Wu

{"title":"Toughness and Thermoresponsive Hydrogel for Sandwich Smart Window with Adaptive Solar Modulation and Energy Saving.","authors":"Huijie Guan, Yinghan Lu, Yijiang You, Shengxiang Gao, Li Liu, Guangfeng Wu","doi":"10.1021/acsami.4c13133","DOIUrl":"https://doi.org/10.1021/acsami.4c13133","url":null,"abstract":"Thermochromic hydrogels with self-regulating solar transmittance are gaining increasing attention due to their significant potential in the fields of smart windows and energy conservation. Smart windows incorporating viscosity-tough hydrogels as an interlayer exhibit enhanced advantages in resisting external forces. In this study, a tough and thermoresponsive composite hydrogel was developed by incorporating poly(N-isopropylacrylamide) nanoparticles (PNIPAM NPs) and W-doped VO2 into a polyacrylamide-agar (PAM-Agar) double network hydrogel. Upon solar irradiation, thermochromism of PNIPAM NPs could regulate the visible light transmittance of the composite hydrogel and the photothermal effect of W-VO2 contributes to the optical regulation and NIR shielding. The smart window, with the composite hydrogel as an interlayer, demonstrates excellent optical modulation capabilities, with a luminous transmittance (Tum(20 °C)) of 86.81%, high light modulation (ΔTum = 78.89%), a high solar modulation (Tsol) of 83.59%, and a lower critical solution temperature (LCST) of 32.6 °C. The composite hydrogel's superior toughness (0.215 MJ/m3) also enhances the impact resistance of the smart window glass. Additionally, the adhesion between the hydrogel and the glass, with a maximum peeling force of up to 151 N/m (attributed to interactions between the amide groups and the silicon hydroxyl groups), was confirmed through a falling ball experiment. Moreover, the hydrogel exhibits a certain degree of thermal insulation, further promoting its utility in energy-saving applications. In conclusion, this study highlights the significant potential of such composite hydrogels in the development of smart windows for energy-efficient buildings.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":null,"pages":null},"PeriodicalIF":8.3,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142306505","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0