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Genes & Diseases 2024年第3期11卷 72-74页

作者： Sha Yang Mei Deng Yunbiao Xiong Bing Xiong junwu fu Jia Wang Jiqin Zhang Guoqiang Han Jian Liu Ying Tan Guizhou University Medical College GuiyangGuizhou 550025China Department of Neurosurgery Guizhou Provincial People's HospitalGuiyangGuizhou 550002China Department of Anesthesiology Guizhou Provincial People's HospitalGuiyangGuizhou 550002China Department of Neurosurgery Chongqing Emergency Medical CenterChongqing400000China

The important role of immunogenic cell death(ICD)in many tumors is increasingly being discovered.However,its mechanisms and potential as a biomarker and therapeutic target in glioblastoma(GBM)have not been well studied.We obtained GBM samples from the Cancer Genome Atlas(TCGA)and Gene Expression Omnibus(GEO)databases,as well as the immunotherapy cohort from the IMvigor210 study.We used unsupervised clustering to obtain two ICDrelated clusters,corresponding to the ICD-low and ICD-high subtypes respectively,and the tumor immune microenvironment and prognosis of the two subtypes were significantly different.

关键词： immune Cancer prognosis

Ribosome-inspired electrocatalysts inducing preferential nucleation and growth of three-dimensional lithium sulfide for high-performance lithium-sulfur batteries

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Journal of Energy Chemistry 2024年第7期94卷 517-526页

作者： Zhen Wu Wenfeng He Jiahui Yang Yunuo Gu Ruiqi Yang Yiran Sun Jiajia Yuan Xin Wang junwu Zhu Yongsheng fu Key Laboratory for Soft Chemistry and functional Materials of Ministry of Education Nanjing University of Science and TechnologyNanjing 210094JiangsuChina School of Energy and Power Engineering Jiangsu UniversityZhenjiang 212013JiangsuChina FEB Res Inst Far East BatteryWuxi 214200JiangsuChina

Nucleation of lithium sulfide(Li_(2)S)induced by electrocatalysts plays a crucial role in mitigating the shut-tle effect.However,short-chain polysulfides on electrocatalysts surfaces tend to re-dissolve into elec-trolytes,delaying Li_(2)S supersaturation and its nucleation.In this study,we draw inspiration from the ribosome-driven protein synthesis process in cells to prepare ultrasmall nitrogen-doped MoS_(2) nanocrys-tals anchored on porous nitrogen-doped carbon networks(N-MoS_(2)-NC)electrocatalysts.Excitedly,the ex-situ SEM demonstrates that ribosome-inspired N-MoS_(2)-NC electrocatalysts induce early nucleation and rapid growth of three-dimensional Li_(2)s during discharge.Theoretical calculations reveal that the Li-s bond length in N-MoS_(2)-Li_(2)S(100)is shorter,and the corresponding interfacial formation energy is lower than in MoS_(2)-Li_(2)S(100).This accelerated conversion of lithium polysulfides to Li_(2)S can enhance the utilization of active substances and inhibit the shuttle effect.This study highlights the potential of ribosome-inspired N-MoS_(2)-NC in improving the electrochemical stability of Li-S batteries,providing valuable insights for future electrocatalyst design.

关键词： Lithium-sulfur batteries Electrocatalysts Nanocrystals Ribosome-inspired Nucleation and growth

Multiscale confinement nitridation in molybdenum carbide for efficient hydrogen production

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Journal of Energy Chemistry 2024年第7期94卷 61-69页

作者： Liming Dai Chenchen Fang Xiaoyuan Zhang Xuefeng Xu Xuanxuan Chen Xinyue Zong Xueming Hu Wenyao Zhang Liang Xue Pan Xiong Yongsheng fu Jingwen Sun junwu Zhu Key Laboratory for Soft Chemistry and functional Materials Ministry of EducationNanjing University of Science and TechnologyNanjing 210094JiangsuChina

The molybdenum carbide(Mo_(2)C)has been regarded as one of the most cost-efficient and stable electrocatalyst for the hydrogen evolution reaction(HER)by the virtue of its Pt-like electronic structures.However,the inherent limitation of high density of empty valence band significantly reduces its catalytic reactivity by reason of strong hydrogen desorption resistance.Herein,we propose a multiscale confinement synthesis method to design the nitrogen-rich Mo_(2)C for modulating the band structure via decomposing the pre-coordination bonded polymer in a pressure-tight tube sealing system.Pre-bonded c/N-Mo in the coordination precursor constructs a micro-confinement space,enabling the homogeneous nitrogenization in-situ happened during the formation of Mo_(2)C.Simultaneously,the evolved gases from the precursor decomposition in tube sealing system establish a macro-confinement environment,preventing the lattice N escape and further endowing a continuous nitridation.Combining the multiscale confinement effects,the nitrogen-rich Mo2C displays as high as 25%N-Mo concentration in carbide lattice,leading to a satisfactory band structure.Accordingly,the constructed nitrogen-rich Mo_(2)C reveals an adorable catalytic activity for HER in both alkaline and acid solution.It is anticipated that the multiscale confinement synthesis strategy presents guideline for the rational design of electrocatalysts and beyond.

关键词： Molybdenum carbide Hydrogen evolution reaction Multiscale confinement synthesis Valence band modulation Nitrogen doping

Modularized sulfur storage achieved by 100% space utilization host for high performance lithium-sulfur batteries

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Chinese Chemical Letters 2024年第4期35卷 237-243页

作者： Jun Jiang Tong Guo Wuxin Bai Mingliang Liu Shujun Liu Zhijie Qi Jingwen Sun Shugang Pan Aleksandr L.Vasiliev Zhiyuan Ma Xin Wang junwu Zhu Yongsheng fu Key Laboratory for Soft Chemistry and functional Materials of Ministry of Education Nanjing University of Science and TechnologyNanjing 210094China Changzhou Institute of Technology Changzhou 213032China Shubnikov Institute of Crystallography Russian Academy of SciencesLeninskii pr.59Moscow 119333Russia Jiangsu Pylon Battery Co. Ltd.Yangzhou 211400China

Popularization of lithium-sulfur batteries(LSBs) is still hindered by shuttle effect and volume expansion.Herein, a new modularized sulfur storage strategy is proposed to solve above problems and accomplished via employing 100% space utilization host material of cobalt loaded carbon nanoparticles derived from ZIF-67. The modular dispersed storage of sulfur not only greatly increases the proportion of active sulfur,but also inhibits the occurrence of volume expansion. Meanwhile, 100% space utilization host material can greatly improve the conductivity of the cathode, provide a larger electrolyte wetting interface and effectively suppress the shuttle effect. Moreover, loaded cobalt particles have high catalytic activity for electrochemical reaction and can effectively improve the redox kinetics. The cell with new cathode host material carbonized at 650 ℃(ZIF-67(650 ℃)) exhibits superior rate performance and can maintain a high specific capacity of 950 m Ah/g after 100 cycles at 0.2 C, showing a good cycle stability.

关键词： Modularized sulfur storage Space utilization Cathode host material ZIF-67 Lithium-sulfur batteries

Metal-organic frameworks derived low-crystalline NiCo_(2)S_(4)/Co_(3)S_(4) nanocages with dual heterogeneous interfaces for high-performance supercapacitors

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Chinese Chemical Letters 2023年第1期34卷 152-158页

作者： Zixin Jia Youning Wang Jiaqi Chen Zhijie Cao Shugang Pan Yan Zhou Jingwen Sun junwu Zhu Xin Wang Yongsheng fu Key Laboratory for Soft Chemistry and functional Materials of Ministry of Education Nanjing University of Science and TechnologyNanjing 210094China Jiangsu Key Laboratory for Chemistry of Low-Dimensional Materials Huaiyin Normal UniversityHuaiyin 223300China Ningxia University Yinchuan 750021China Changzhou Institute of Technology Changzhou 213032China

Nickel cobalt bimetallic heterogeneous sulfides are attractive battery-type materials for electrochemical energy storage.However,the precise synthesis of electrode materials that integrate highly efficient ions/electrons diffusion with abundant charge transfer channels has always been challenging.Herein,an effective and concise controllable hydrothermal approach is reported for tuning the crystalline and integrated structures of MOF-derived bimetallic sulfides to accelerate the charge transfer kinetics,and thus enabling rich Faradaic redox reaction.The as-obtained low-crystalline heterogeneous NiCo_(2)S_(4)/Co_(3)S_(4)nanocages exhibit a high specific capacity(1023 C/g at 1 A/g),remarkable rate performance(560 C/g at 10A/g),and outstanding cycling stability(89.6%retention after 5000 cycles).furthermore,hybrid supercapacitors fabricated with NiCo_(2)S_(4)/Co_(3)S_(4)and nitrogen-doped reduced graphene oxide display an outstanding energy density of 40.8 Wh/kg at a power density of 806.3 W/kg,with an excellent capacity retention of 88.3%after 10000 charge-discharge cycles.

关键词： Metal-organic frameworks Nickel cobalt heterogeneous sulfides Low-crystalline nanostructure High-performance supercapacitors High energy density

Supramolecular assembly-derived carbon-nitrogen-based functional materials for photo/electrochemical applications: progress and challenges

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National Science Open 2023年第4期2卷 1-37页

作者： Fanglei Yao Chenchen Fang Junjie Cui Liming Dai Xiaoyuan Zhang Liang Xue Pan Xiong Yongsheng fu Wenyao Zhang Jingwen Sun junwu Zhu Key Laboratory for Soft Chemistry and functional Materials Ministry of EducationNanjing University of Science and TechnologyNanjing 210094China

Supramolecular chemistry during the synthesis of carbon-nitrogen-based materials has recently experienced a renaissance in the arena of photocatalysis and electrocatalysis.In this review,we start with the discussion of supramolecular assemblies-derived carbon-nitrogen-based materials’regulation from the aspect of morphology,chemical composition,and micro/nanostructural control.Afterwards the recent advances of these materials in energy and environment related applications,including degradation of pollutants,water splitting,oxygen reduction reactions,CO_(2) reduction reactions along with organic synthesis are summarized.The correlations between the structural features and physicochemical properties of the carbonnitrogen-based materials and the specific catalytic activity are discussed in depth.By highlighting the opportunities and challenges of supramolecular assembly strategies,we attempt an outlook on possible future developments for highly efficient carbon-based photo/electrocatalysts.

关键词： supramolecular assembly carbon carbon nitride photocatalysis electrocatalysis

非贵金属/碳氮复合材料电催化析氧反应的研究进展

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无机材料学报 2022年第2期37卷 163-172页

作者：付永胜毕敏李春孙敬文汪信朱俊武南京理工大学软化学与功能材料教育部重点实验室南京210094

析氧反应(OER)是一种复杂的四电子转移反应,其动力学缓慢、所需能量高,制约了电解水制氢等新型能源技术的发展。近年来,非贵金属复合材料因其优异的催化活性以及相比于贵金属基催化剂的成本优势而受到广泛关注。本文概述了这一研究领域... 详细信息

析氧反应(OER)是一种复杂的四电子转移反应,其动力学缓慢、所需能量高,制约了电解水制氢等新型能源技术的发展。近年来,非贵金属复合材料因其优异的催化活性以及相比于贵金属基催化剂的成本优势而受到广泛关注。本文概述了这一研究领域的最新进展,首先简要介绍析氧反应的机理以及材料催化性能的评价方法,重点关注非贵金属/碳氮复合材料析氧电催化剂,并且将非贵金属/碳氮复合材料分为金属单质/碳氮复合材料、单原子/碳氮复合材料、合金/碳氮复合材料、金属氧化物/碳氮复合材料,从制备方法和催化活性出发,探究氮掺杂碳材料在催化剂结构和催化剂性能中的作用,总结分析了几类非贵金属/碳氮复合材料在电催化析氧反应中的研究进展。最后,针对非贵金属/碳氮复合材料目前存在的问题和未来发展方向提出了建议。

关键词：析氧反应非贵金属复合材料电催化综述

基于不同切样角度的高温原状多年冻土直剪力学特性试验研究

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成都理工大学学报（自然科学版） 2022年第5期49卷 616-622,640页

作者：朱锋盼赵晓东李俊虎付俊武中国矿业大学深部岩土力学与地下工程国家重点实验室江苏徐州221116 金华职业技术学院浙江金华321017 中建隧道建设有限公司重庆401320

利用原状多年冻土在不同切样角度下的直剪试验,探讨-2℃条件下青藏地区2种不同土性(粉土、粉质黏土)冻土的直剪力学特性。结果表明:原状冻结粉土含冰量变化较小,内部为层状构造,而原状冻结粉质黏土含冰量变化较大,可以看到冻土中有冰块... 详细信息

利用原状多年冻土在不同切样角度下的直剪试验,探讨-2℃条件下青藏地区2种不同土性(粉土、粉质黏土)冻土的直剪力学特性。结果表明:原状冻结粉土含冰量变化较小,内部为层状构造,而原状冻结粉质黏土含冰量变化较大,可以看到冻土中有冰块;原状冻结粉土、原状冻结粉质黏土剪切位移(Δl)-剪应力(τ)曲线表现为硬化型;原状粉质黏土随着含冰量增加呈现脆性破坏的趋势;原状冻结粉土的抗剪强度受剪切角度的影响较大,在200 kPa法向应力作业下,不同剪切角度下得到的原状冻结粉土抗剪强度τ_(max)是τ_(min)的1.22倍。通过理论分析可知,在层理面上开展直剪试验,其抗剪强度最小;因此,对于高温原状多年冻土的抗剪强度的取值应考虑切样角度的影响。

关键词：切样角度高温原状多年冻土直剪试验抗剪强度

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环氧化丁基橡胶的合成与表征

高分子学报 2022年第2期53卷 185-192页

作者：吴君崔百川王岩石艳任学斌徐宏德刘振学郝福兰张立群北京化工大学北京市新型高分子材料制备与加工重点实验室北京100029 黄河三角洲京博化工研究院有限公司滨州256600 山东京博中聚新材料有限公司滨州256600

以正己烷为溶剂、间氯过氧苯甲酸(mCPBA)为环氧化试剂对丁基橡胶(IIR)进行环氧化改性研究,考察了原料配比、反应温度、胶液浓度等反应条件对环氧化反应的影响,并对反应过程中发生的副反应进行了探究.采用核磁共振氢谱(1H-NMR)对合成的... 详细信息

以正己烷为溶剂、间氯过氧苯甲酸(mCPBA)为环氧化试剂对丁基橡胶(IIR)进行环氧化改性研究,考察了原料配比、反应温度、胶液浓度等反应条件对环氧化反应的影响,并对反应过程中发生的副反应进行了探究.采用核磁共振氢谱(1H-NMR)对合成的环氧化丁基橡胶(EIIR)的结构进行了表征,并对环氧化度进行了定量计算.确定了最优的反应条件:胶液浓度为15%、双键与mCPBA的摩尔比为1∶1.1、40~45℃下反应45 min,之后用NaOH水溶液洗涤除酸,能够实现IIR中异戊二烯单元的完全环氧化,且无副反应.利用示差扫描量热仪(DSC)和热重分析仪(TGA)表征了EIIR的热性能,改性后IIR的玻璃化转变温度(Tg)和热分解温度均有小幅度提高.此外,EIIR还具有十分良好的储存稳定性.

关键词：丁基橡胶环氧化间氯过氧苯甲酸开环反应

氢键有机框架材料在电化学能源存储和转换中的研究进展

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科学通报 2023年第25期68卷 3335-3352页

作者：方晨晨许雪凤张校源代黎明姚方磊张文耀付永胜孙敬文朱俊武南京理工大学软化学与功能材料教育部重点实验室南京210094

作为一种新型的多孔材料,氢键有机框架(hydrogen-bonded organic frameworks,HOFs)结构因其丰富的孔道分布、可控的晶体构型以及易于调节的分子组成而表现出诸多优异的电化学特性,如快速的离子传输、特异性的离子筛分、可观的电化学活... 详细信息

作为一种新型的多孔材料,氢键有机框架(hydrogen-bonded organic frameworks,HOFs)结构因其丰富的孔道分布、可控的晶体构型以及易于调节的分子组成而表现出诸多优异的电化学特性,如快速的离子传输、特异性的离子筛分、可观的电化学活性面积、高暴露的催化活性位点等.这些特性促使研究者越来越多地关注其在电化学能源存储和转换技术中的应用,是能源领域研究的前沿和热点.尽管这些HOFs相关材料的结构和组成各不相同,总体上却可以分为HOFs和HOFs衍生物两大类.本文详细地介绍了HOFs及其衍生物作为电极材料或电催化剂在电化学领域,包括可充电离子电池、电化学超级电容器、电催化析氢、电催化析氧和氧还原反应中的应用原理与最新研究进展.在此基础上,重点阐述了HOFs相关材料的纳米形貌、晶体结构、孔道结构和分子组成对其电化学性能的影响,总结了克服HOFs相关材料氢键骨架稳定性和导电性差的相关方法,凝练了它们在该领域发展中的优势和挑战.基于上述讨论,希望对HOFs相关材料在电化学能源存储和转换技术中的发展提供新的研究方向.

关键词：氢键有机框架锂/钠离子电池超级电容器析氧反应氧还原反应析氢反应