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Unlocking high-efficiency oxygen evolution reaction through Co-N coordination engineering in Co@N-doped porous carbon core–shell nanoparticles

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Nano Research 2024年第8期17卷 7068-7076页

作者： Shucheng Liu Yu Shuai Xiaosi Qi zhao ding Yi Liu College of Big Data and Information Engineering Guizhou UniversityGuiyang 550025China College of Physics Guizhou Province Key Laboratory for Photoelectrics Technology and ApplicationGuizhou UniversityGuiyang 550025China

Modulation of metal sites coordination can significantly refine the electronic architecture of catalysts,thereby improving their catalytic *** work successfully developed a core–shell Co@N-doped porous carbon(Co@NC)catalyst by pyrolyzing the COF/MOF(IISERP-COF3/ZIF-67)composite in an inert *** Co@NC catalyst exhibited impressive oxygen evolution reaction(OER)performance,with a small overpotential of 304 mV and a modest Tafel slope of 88.6 mV·dec^(−1) in a 1 M KOH,alongside remarkable stability,maintaining 98.5%of its activity over 13 *** role of IISERP-COF3 was pivotal in preventing Co atom aggregation during the ZIF-67 pyrolysis,which facilitated the creation of mesopores for enhanced mass transport and ***,it effectively modulated the Co-N coordination to fine-tune the electronic structure,thereby optimizing the catalyst's capacity for adsorption of intermediates and boosting its intrinsic *** functional theory(DFT)studies corroborate that the exceptional OER efficiency of Co@NC can be linked to the enhanced Co-N coordination,optimizing the localized electronic structure at the Co active *** study not only proposes an innovative approach for optimizing COF/MOF as effective electrocatalysts but also clears the path for the emergence of affordable,high-performance alternatives to precious metal-based catalysts,marking a significant advancement in sustainable energy technologies.

关键词： covalent organic framework(COF) metal-organic framework(MOF) core-shell structure catalysts oxygen evolution reaction

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Early results of the integrative epigenomic-transcriptomic landscape of colorectal adenoma and cancer

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World Journal of Gastrointestinal Oncology 2024年第2期16卷 414-435页

作者： You-Wang Lu zhao-Li ding Rui Mao Gui-Gang zhao Yu-Qi He Xiao-Lu Li Jiang Liu Department of Dermatology and Venereology The First Affiliated Hospital of Kunming Medical UniversityKunming 650032Yunnan ProvinceChina Kunming Biological Diversity Regional Center of Large Apparatus and Equipments Public Technical Service CenterKunming Institute of ZoologyKunming 650223Yunnan ProvinceChina School of Stomatology Kunming Medical UniversityKunming 650500Yunnan ProvinceChina Genome Center of Biodiversity Kunming Institute of ZoologyChinese Academy of ScienceKunming 650223Yunnan ProvinceChina Department of Reproduction and Genetics The First Affiliated Hospital of Kunming Medical UniversityKunming 650032Yunnan ProvinceChina

BACKGROUND Aberrant methylation is common during the initiation and progression of colorectal cancer(CRC),and detecting these changes that occur during early adenoma(ADE)formation and CRC progression has clinical *** To identify potential DNA methylation markers specific to ADE and *** Here,we performed SeqCap targeted bisulfite sequencing and RNA-seq analysis of colorectal ADE and CRC samples to profile the epigenomic-transcriptomic *** Comparing 22 CRC and 25 ADE samples,global methylation was higher in the former,but both showed similar methylation patterns regarding differentially methylated gene positions,chromatin signatures,and repeated ***-grade CRC tended to exhibit elevated methylation levels in gene promoter regions compared to those in low-grade *** with RNA-seq gene expression data,we identified 14 methylation-regulated differentially expressed genes,of which only AGTR1 and NECAB1 methylation had prognostic *** Our results suggest that genome-wide alterations in DNA methylation occur during the early stages of CRC and demonstrate the methylation signatures associated with colorectal ADEs and CRC,suggesting prognostic biomarkers for CRC.

关键词： Colorectal cancer Epigenomic alteration Transcriptome Methylation-regulated differentially expressed genes

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Small molecule deoxynyboquinone triggers alkylation and ubiquitination of Keap1 at Cys489 on Kelch domain for Nrf2 activation and inflammatory therapy

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Journal of Pharmaceutical Analysis 2024年第3期14卷 401-415页

作者： Ke-Gang Linghu Tian Zhang Guang-Tao Zhang Peng Lv Wen-Jun Zhang Guan-ding zhao Shi-Hang Xiong Qiu-Shuo Ma Ming-Ming zhao Meiwan Chen Yuan-Jia Hu Chang-Sheng Zhang Hua Yu State Key Laboratory of Quality Research in Chinese Medicine Institute of Chinese Medical SciencesUniversity of MacaoMacao SARChina Macao Centre for Research and Development in Chinese Medicine Institute of Chinese Medical SciencesUniversity of MacaoMacao SARChina Key Laboratory of Tropical Marine Bio-resources and Ecology Guangdong Key Laboratory of Marine Materia MedicaRNAM Center for Marine MicrobiologySouth China Sea Institute of OceanologyChinese Academy of SciencesGuangzhou510301China State Key Laboratory of Functions and Applications of Medicinal Plants&School of Pharmaceutical Sciences Guizhou Medical UniversityGuiyang550025China

Activation of nuclear factor erythroid 2-related factor 2(Nrf2)by Kelch-like ECH-associated protein 1(Keap1)alkylation plays a central role in anti-inflammatory ***,activators of Nrf2 through alkylation of Keap1-Kelch domain have not been ***(DNQ)is a natural small molecule discovered from marine *** current study was designed to investigate the anti-inflammatory effects and molecular mechanisms of DNQ via alkylation of *** exhibited significant anti-inflammatory properties both in vitro and in *** pharmacophore responsible for the anti-inflammatory properties of DNQ was determined to be theα,β-unsaturated amides moieties by a chemical reaction between DNQ and *** exerted anti-inflammatory effects through activation of Nrf2/ARE ***1 was demonstrated to be the direct target of DNQ and bound with DNQ through conjugate addition reaction involving *** specific alkylation site of DNQ on Keap1 for Nrf2 activation was elucidated with a synthesized probe in conjunction with liquid chromatography-tandem mass *** triggered the ubiquitination and subsequent degradation of Keap1 by alkylation of the cysteine residue 489(Cys489)on Keap1-Kelch domain,ultimately enabling the activation of *** findings revealed that DNQ exhibited potent anti-inflammatory capacity throughα,β-unsaturated amides moieties active group which specifically activated Nrf2 signal pathway via alkylation/ubiquitination of Keap1-Kelch domain,suggesting the potential values of targeting Cys489 on Keap1-Kelch domain by DNQ-like small molecules in inflammatory therapies.

关键词： Deoxynyboquinone Anti-inflammation Target Keap1/Nrf2 Alkylation Ubiquitination

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Three-dimensional visualization technology for guiding one-step percutaneous transhepatic cholangioscopic lithotripsy for the treatment of complex hepatolithiasis

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World Journal of Gastroenterology 2024年第28期30卷 3393-3402页

作者： Yong-Qing Ye Ya-Wen Cao Rong-Qi Li En-Ze Li Lei Yan zhao-Wei ding Jin-Ming Fan Ping Wang Yi-Xiang Wu Department of Hepatobiliary Surgery The Second People’s Hospital of FoshanFoshan 528000Guangdong ProvinceChina Department of Emergency Medicine Biomedical Innovation CenterThe Sixth Affiliated HospitalSun Yat-sen UniversityGuangzhou 510655Guangdong ProvinceChina Department of Hepatobiliary Surgery Foshan Hospital of Traditional Chinese MedicineFoshan 528000Guangdong ProvinceChina Department of Hepatobiliary Surgery The First Affiliated Hospital of Guangzhou Medical UniversityGuangzhou 510282Guangdong ProvinceChina Department of Gastrointestinal Surgery The First Affiliated Hospital of Guangzhou Medical UniversityGuangzhou 510120Guangdong ProvinceChina

BACKGROUND Biliary stone disease is a highly prevalent condition and a leading cause of hospitalization *** with associated strictures has high residual and recurrence rates after traditional multisession percutaneous transhepatic cholangioscopic lithotripsy(PTCSL).AIM To study one-step PTCSL using the percutaneous transhepatic one-step biliary fistulation(PTOBF)technique guided by three-dimensional(3D)*** This was a retrospective,single-center study analyzing,140 patients who,between October 2016 and October 2023,underwent one-step PTCSL for *** patients were divided into two groups:The 3D-PTOBF group and the PTOBF *** clearance on choledochoscopy,complications,and long-term clearance and recurrence rates were *** Age,total bilirubin,direct bilirubin,Child-Pugh class,and stone location were similar between the 2 groups,but there was a significant difference in bile duct strictures,with biliary strictures more common in the 3D-PTOBF group(P=0.001).The median follow-up time was 55.0(55.0,512.0)*** immediate stone clearance ratio(88.6%vs 27.1%,P=0.000)and stricture resolution ratio(97.1%vs 78.6%,P=0.001)in the 3D-PTOBF group were significantly greater than those in the PTOBF *** complication(8.6%vs 41.4%,P=0.000)and stone recurrence rates(7.1%vs 38.6%,P=0.000)were significantly lower in the 3D-PTOBF *** Three-dimensional visualization helps make one-step PTCSL a safe,effective,and promising treatment for patients with complicated primary *** perioperative and long-term outcomes are satisfactory for patients with complicated primary *** minimally invasive method has the potential to be used as a substitute for hepatobiliary surgery.

关键词： Hepatolithiasis One-step percutaneous transhepatic cholangioscopic lithotripsy Biliary disease Three-dimensional visualization Clinical efficacy

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The future path to sutureless surgery:Self–adhesive tough hydrogel

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Science Bulletin 2024年第15期69卷 2307-2310页

作者： Lei Xiang ding zhao Yihan Li Qimanguli Saiding Wenguo Cui Department of Orthopaedics Shanghai Key Laboratory for Prevention and Treatment of Bone and Joint DiseasesShanghai Institute of Traumatology and OrthopaedicsRuijin HospitalShanghai Jiao Tong University School of MedicineShanghai 200025China

Surgical sutures serve as foundational elements in surgical procedures,facilitating wound closure,exudation minimization,infection prevention,structural support maintenance,and healing *** classification of traditional surgical suturing methods is intricate,and contingent upon variables such as tissue type,wound morphology,and desired healing outcomes.

关键词： healing wound prevention

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GaAsBi半导体材料的制备及应用研究进展

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人工晶体学报 2024年第1期53卷 25-37页

作者：马玉麟郭祥丁召贵州大学大数据与信息工程学院贵阳550025 贵州省微纳电子与软件技术重点实验室贵阳550025 半导体功率器件可靠性教育部工程研究中心贵阳550025

稀铋Ⅲ-Ⅴ半导体材料在电子和光电子领域具有广泛的应用前景,其制备方法主要有分子束外延法(MBE)和金属有机物气相外延法(MOVPE)。本文聚焦于具有较大带隙收缩、温度不敏感以及强自旋轨道分裂等特殊物理特性的GaAs_(x)Bi_(1-x)半导体材... 详细信息

稀铋Ⅲ-Ⅴ半导体材料在电子和光电子领域具有广泛的应用前景,其制备方法主要有分子束外延法(MBE)和金属有机物气相外延法(MOVPE)。本文聚焦于具有较大带隙收缩、温度不敏感以及强自旋轨道分裂等特殊物理特性的GaAs_(x)Bi_(1-x)半导体材料,对其制备方法和研究进展进行了综述。研究人员对GaAsBi材料的研究主要集中在薄膜、多量子阱、纳米线和量子点材料的制备。在薄膜材料方面,侧重于研究制备工艺条件对GaAsBi薄膜的影响,例如低衬底温度、低生长速率和非常规的Ⅴ/Ⅲ束流比;在多量子阱材料方面,采用双衬底温度技术有效减少Bi偏析问题;对于纳米线和量子点材料,金属Bi作为表面活性剂可以改善材料的形貌和光学性能。然而,目前在该材料研究和应用方面仍存在挑战,如薄膜材料的结晶质量恶化和金属Bi分凝团聚,以及量子点材料中Bi的均匀性和形成机制的争议。解决这些问题对于提高GaAs_(x)Bi_(1-x)半导体材料的质量和促进器件发展具有重要意义。

关键词：稀铋Ⅲ-Ⅴ半导体材料 GaAsBi薄膜多量子阱材料量子点材料 MBE MOVPE

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揭示配体拓扑结构对Fe-Nx-C单原子催化剂表面氧还原反应中间体吸附的影响（英文）

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Chinese Journal of Catalysis 2024年第4期59卷 214-224页

作者：吴德贵熊孝根赵中栋宋树芹丁朝斌中山大学化学工程与技术学院中山大学中法核工程与技术学院中山大学材料科学与技术学院

过渡金属单原子氮掺杂碳催化剂（TM-N-CSAC）因其更高的金属原子效率而被认为是提升氧还原反应（ORR）效率的重要途径.TM-N-CSAC反应中心的活性与配体结构密切相关,构建基于配体结构的ORR活性描述符是高效设计高催化活性单原子催化剂的... 详细信息

过渡金属单原子氮掺杂碳催化剂（TM-N-CSAC）因其更高的金属原子效率而被认为是提升氧还原反应（ORR）效率的重要途径.TM-N-CSAC反应中心的活性与配体结构密切相关,构建基于配体结构的ORR活性描述符是高效设计高催化活性单原子催化剂的关键.然而目前大多配体描述符基于催化剂的综合表观性质,如OH吸附能和金属中心d带中心等,其获取仍需进行额外计算,不利于通过配体结构快速推测反应活性;而目前基于配体结构拓扑参数,如金属中心原子及其配位原子属性、数量等设计的描述符存在对催化活性的描述较差或仅适用于特定配体等问题.解决该难题的关键在于理清OH与TM-N-C SAC成键的微观机制.本文全面考察了ORR中间体OH在21种具有不同氮原子数量、位置以及不同配体尺寸的卟啉型FeNxC SAC表面上的吸附机制.对有限尺寸卟啉型Fe-Nx-C （x=0-4）SAC模型上OH吸附的密度泛函理论计算结果表明, OH吸附能与SAC的配位氮原子的数量并不线性相关,且受氮原子排布方式的影响.利用能量分解分析（EDA）将OH与SAC的成键作用分解,重点讨论氮的掺入对静电作用、泡利排斥作用和轨道作用的影响.针对静电作用, Bader分析与电荷密度差值分析结果表明,氮的掺入一方面将电荷向配位原子上聚集,且配位原子上电荷数随氮原子数量增加而线性增加;另一方面大幅增强铁-配体键（Fe-L）的离子性,减少铁与配体间的电子密度,提高铁中心电子能量,并从而改变静电作用能量.对于泡利排斥作用,其影响因素与静电作用类似,因而作用强度与静电作用强度呈较好线性关系.对于轨道作用,结合扩展过渡态-化学价的自然轨道（ETS-NOCV）和电子定域化（LOL-π）等综合分析发现,氮原子的掺入破坏了配体的离域π键,从而影响OH与配体的轨道在成键时的相互作用.此外,对配体大小影响的研究表明,配体边缘原子仅当出现在包含配位原子的环上时才对OH与SAC成键有较大影响,这充分证明了OH吸附这一过程的局域性.综上,本文提供了Fe-N-C型SAC上完整的OH吸附键形成机制,强调了配位原子及其近邻原子对吸附活性的影响,为构建基于SAC拓扑特征的ORR活性描述符,实现SAC配体的快速筛选提供参考.

关键词：单原子催化剂氧还原反应配体拓扑结构能量分解分析密度泛函理论

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Behavior of exciton in direct−indirect band gap Al_(x)Ga_(1−x)As crystal lattice quantum wells

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Journal of Semiconductors 2024年第3期45卷 64-70页

作者： Yong Sun Wei Zhang Shuang Han Ran An Xin-Sheng Tang Xin-Lei Yu Xiu-Juan Miao Xin-Jun Ma Xianglian Pei-Fang Li Cui-Lan zhao zhao-Hua ding Jing-Lin Xiao Institute of Condensed Matter Physics Inner Mongolia Minzu UniversityTongliao 028043China College of Physics and Electronic Information Inner Mongolia Minzu UniversityTongliao 028043China

Excitons have significant impacts on the properties of *** exhibit significantly different properties when a direct semiconductor turns in to an indirect one by *** variational method is also found to influence the study of exciton ground state energy and ground state binding energy in Al_(x)Ga_(1−x)As semiconductor spherical quantum *** Al_(x)Ga_(1−x)As is considered to be a direct semiconductor at AI concentration below 0.45,and an indirect one at the concentration above *** regards to the former,the ground state binding energy increases and decreases with AI concentration and eigenfrequency,respectively;however,while the ground state energy increases with AI concentration,it is marginally influenced by *** the other hand,considering the latter,while the ground state binding energy increases with AI concentration,it decreases with eigenfrequency;nevertheless,the ground state energy increases both with AI concentration and ***,for the better practical performance of the semiconductors,the properties of the excitons are suggested to vary by adjusting AI concentration and eigenfrequency.

关键词： exciton effects aluminum gallium arsenide crystal direct band gap semiconductor indirect band gap semiconductor

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稀土元素(La、Eu、Ho)掺杂单层WSe_(2)的第一性原理研究

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功能材料 2024年第2期55卷 2155-2160,2167页

作者：姜冠戈江玉琪郭祥丁召贵州大学大数据与信息工程学院贵阳550025 贵州省微纳电子与软件技术重点实验室贵阳550025 半导体功率器件可靠性教育部工程研究中心贵阳550025

单层二硒化钨(WSe_(2))是一种具有良好的热稳定性、电子运输和大面积可扩展性的优秀特性。基于密度泛函理论,利用第一性原理计算研究了稀土元素(La、Eu、Ho)掺杂单层WSe_(2)的结构、电学性质和光学性质。采用稀土元素(La、Eu、Ho)掺杂... 详细信息

单层二硒化钨(WSe_(2))是一种具有良好的热稳定性、电子运输和大面积可扩展性的优秀特性。基于密度泛函理论,利用第一性原理计算研究了稀土元素(La、Eu、Ho)掺杂单层WSe_(2)的结构、电学性质和光学性质。采用稀土元素(La、Eu、Ho)掺杂使单层WSe_(2)呈现P型导电传输特性,增强了导电性能,展现半金属特性。此外,La、Eu、Ho掺杂后,提高了单层WSe_(2)在红外光区的光探测能力和对可见光的利用率,在深紫外区域也具有应用潜力。研究结果证明了La、Eu、Ho掺杂单层WSe_(2)的电学性质、光学性质和扩大其应用方面的重要性。

关键词：单层二硒化钨第一性原理计算掺杂光学性质

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基于深度学习、小波变换和可见光谱的茶树冻害程度评估

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光谱学与光谱分析 2024年第1期44卷 234-240页

作者：李赫王玉范凯毛艺霖丁仕波宋大鹏王梦琪丁兆堂山东省农业科学院茶叶研究所山东济南250108 青岛农业大学茶叶研究所山东青岛266109 日照市农业科学研究院茶叶研究所山东日照276827

茶树冻害鉴定是评价茶树抗逆性、指导茶园越冬管理的基础。茶树冻害鉴定的传统方法主要通过人工观察茶树叶片的冻害数量和冻害程度,存在准确率低,效率低,主观性强等缺点。提出一种基于深度学习、小波变换和可见光谱的茶树冻害程度评估... 详细信息

茶树冻害鉴定是评价茶树抗逆性、指导茶园越冬管理的基础。茶树冻害鉴定的传统方法主要通过人工观察茶树叶片的冻害数量和冻害程度,存在准确率低,效率低,主观性强等缺点。提出一种基于深度学习、小波变换和可见光谱的茶树冻害程度评估框架。首先,采集了1 000张茶树受冻后的树冠图像,并且按照4∶1分为训练集和测试集,并对训练集图像的冻害叶片进行标注。其次,采用Faster R-CNN网络对茶树的冻害叶片进行识别提取,并且分别选择了AlexNet、 VGG19和ResNet50三种特征提取器,选择鲁棒性最高的特征提取器作为主干网络。然后,将提取到的茶树冻害叶片图像进行小波变换增强处理,从而得到了一张低频率和三张高频率的图像。将小波变换处理后的图像和未经小波变换处理的图像分别输入到VGG16、 SVM、 AlexNet、 ResNet50等网络对冻害叶片进行分级,比较四种网络的分类性能。根据冻害叶片的数量、冻害叶片的程度,不同冻害程度叶片的权重系数,对茶树受冻程度打分,从而对茶树整体的冻害程度进行评估。结果表明:(1)基于ResNet50的Faster R-CNN模型提取茶树冻害叶片的性能最好,其查准率为93.33%,查全率为92.57%,高于VGG19和AlexNet作为主干网络的识别性能,可以确保大多数的冻害叶片都能被提取出来,并为叶片的冻害程度进一步分级提供基础。(2)VGG16模型分类不同冻害程度的叶片的整体准确率为89%,高于其他模型(SVM、 AlexNet、 ResNet50)的整体分类准确率,表明VGG16模型具有较高的鲁棒性。(3)小波变换处理后的冻害叶片图像与未经小波变换处理后的冻害叶片相比较,能提升模型的整体分类准确率2%~6%。说明小波变换增强技术可以提高网络的准确率。因此,本实验框架可以准确和高效地将茶树冻害叶片进行分级,对于茶园冻害程度的评估具有重要价值,为北方茶园的越冬防护提供技术支撑。

关键词：茶树冻害叶片 Faster R-CNN VGG16 小波变换

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