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Unraveling the catalytic redox mechanism of lithium–sulfur batteries through advanced in-situ/operando characterizations

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Science China Chemistry 2024年

作者： Pan Zeng Cheng Yuan Bin Su Genlin Liu jiechang gao Kun Yang Qingyuan Wang Liang Zhang Institute for Advanced Study School of Mechanical Engineering Chengdu University Institute of Functional Nano & Soft Materials (FUNSOM) Soochow University Dyson School of Design Engineering Imperial College London

Accelerating the redox conversion of lithium polysulfides(LiPSs) with electrocatalysts has been regarded as an effective avenue to surmount the shuttle effect and realize high-performance lithium–sulfur(Li–S) batteries. However, the complicated reaction process, especially the real-time evolution of sulfur-containing species and electrocatalysts under working conditions, has brought great difficulties in the explicit understanding of reaction mechanism of Li–S batteries, thereby severely hampering the design of highly efficient electrocatalysts. Therefore, a crucial prerequisite for correctly identifying the reaction mechanism is an in-depth analysis of the dynamic evolution of reaction intermediates and their structure-performance relationships. In this review,we comprehensively summarized the most recent progress in the dynamic behaviors of LiPSs and electrocatalysts of Li–S batteries under working conditions in conjunction with closely related in-situ/operando characterizations to recognize the realtime evolution of phase, composition, and atomic/electronic structure, thereby unraveling the corresponding catalytic mechanism. In addition, the major challenges and unexplored issues of catalytic conversion of LiPSs were summarized and discussed, aiming to provide perspectives into the development of highly efficient electrocatalysts in Li–S chemistry. Based on this review, we believe that reasonable regulation of reconstruction behaviors can achieve satisfactory electrocatalysts with high catalytic activity, accelerating the development of green energy.

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Recent progress in electronic modulation of electrocatalysts for high-efficient polysulfide conversion of Li-S batteries

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Chinese Journal of Catalysis 2022年第12期43卷 2946-2965页

作者： Pan Zeng Cheng Yuan Genlin Liu jiechang gao Yanguang Li Liang Zhang Institute of Functional Nano&Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials&DevicesSoochow UniversitySuzhou 215123JiangsuChina

With the merits of high energy density,environmental friendliness,and cost effectiveness,lithium-sulfur(Li-S)batteries are considered as one of the most promising next-generation electrochemical storage ***,the notorious polysulfide shuttle effect,which results in low active material utilization and serious capacity fading,severely impedes the practical application of Li-S *** various electrocatalysts to improve the polysulfide redox kinetics has recently emerged as a promising strategy to address the shuttle ***,the electronic structure of the electrocatalysts plays a decisive role in determining the catalytic activity to facilitate the polysulfide ***,reasonably modulating the electronic structure of electrocatalysts is of paramount significance for improving the electrochemical performance of Li-S ***,a comprehensive overview of the fascinating strategies to tailor the electronic structure of electrocatalysts for Li-S batteries is presented,including but not limited to vacancy engineering,heteroatom doping,single atom doping,band regulation,alloying,and heterostructure *** future perspectives and challenges are also proposed for designing high-efficient electrocatalysts to construct high-energy-density and long-lifetime Li-S batteries.

关键词： Lithium-sulfur batteries Catalytic effect Electronic modification Shuttle effect Redox kinetics

Downregulation effects of beta-elemene on the levels of plasma endotoxin,serum TNF-alpha,and hepatic CD14 expression in rats with liver fibrosis

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Frontiers of Medicine 2011年第1期5卷 101-105页

作者： Jianguo LIU Zhe ZHANG jiechang gao Jiwen XIE Lin YANG Shenjun HU Department of Traditional Chinese Medicine Union HospitalTongji Medical CollegeHuazhong University of Science&TechnologyWuhan 430022China Department of Oncology The Second Staff Hospital of Wuhan Iron and Steel(Group)Corp.Wuhan 430085China

It has been demonstrated thatβ-elemene could protect against carbon tetrachloride(CCl_(4))-induced liver fibrosis in our laboratory work,and the aim of this paper is to reveal the protective mechanisms ofβ-*** hepatic fibrosis experimental model was induced by the hypodermical injection of CCl_(4) in Wistar male rats.β-elemene was intraperitoneally administered into rats for 8 weeks(0.1 mL/100 g bodyweight per day),and plasma endotoxin content was assayed by *** serum TNF-αlevel was detected using radioactive ***14 expression in rat livers was measured by immunohistochemistry and Western *** results showed thatβ-elemene can downregulate the levels of plasma endotoxins,serum TNF-α,and hepatic CD14 expression in rats with liver fibrosis.β-elemene plays an important role in downregulating the lipopolysaccharide signal transduction pathway,a significant pathway in hepatic fibrosis development.

关键词： liver fibrosis beta-elemene endotoxin CD14

C(18)DMAAC共聚物暂堵剂的制备及其性能

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石油化工 2016年第4期45卷 461-466页

作者：郜杰昌张定军冯照喧兰州理工大学材料科学与工程学院甘肃兰州730050 兰州理工大学省部共建有色金属先进加工与再利用国家重点实验室甘肃兰州730050

以丙烯酰胺(AM)、丙烯酸(AA)、马来酸酐(MAH)、十八烷基二甲基烯丙基氯化铵(C(18)DMAAC)为原料,采用溶液聚合法合成了共聚物暂堵剂AM-C18-AA和AM-C18-MAH。利用FTIR和SEM等手段表征了共聚物的结构和形貌,并研究了吸水率和溶胀动力学。... 详细信息

以丙烯酰胺(AM)、丙烯酸(AA)、马来酸酐(MAH)、十八烷基二甲基烯丙基氯化铵(C(18)DMAAC)为原料,采用溶液聚合法合成了共聚物暂堵剂AM-C18-AA和AM-C18-MAH。利用FTIR和SEM等手段表征了共聚物的结构和形貌,并研究了吸水率和溶胀动力学。表征结果显示,C(18)DMAAC的引入使共聚物分子链中增加了疏水链段,赋予共聚物更规则的形貌。实验结果表明,AM-C18-AA的吸水及溶胀性能优异,最高吸水率(蒸馏水)达360 g/g;C(18)DMAAC的加入提高了AM-C18-MAH的耐盐性能,在盐水中的吸水率最大为62 g/g。两种共聚物均具有较快的吸水速率,并能在较短时间内达到溶胀平衡。AM-C18-AA在碱性溶液中的增黏效应使其更符合压裂作业需求,适合用作聚合物暂堵剂。

关键词：暂堵剂离子型单体溶液聚合吸水率黏度变化

AM-AA共聚物/SA复合材料小球堵水剂的研究

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石油化工 2014年第11期43卷 1315-1318页

作者：瞿朝云张定军郜杰昌吴有智冯照喧兰州理工大学材料科学与工程学院省部共建有色金属先进加工与再利用国家重点实验室甘肃兰州730050

以丙烯酰胺(AM)、中和度为70%的丙烯酸(AA)和海藻酸钠(SA)为原料,过硫酸钾(KPS)为引发剂,在水溶液聚合法合成AM-AA共聚物/SA复合材料的基础上,添加淀粉和交联剂硝酸铝,采用造粒工艺制备了一种新型堵水剂AM-AA共聚物/SA复合材料小球(粒... 详细信息

以丙烯酰胺(AM)、中和度为70%的丙烯酸(AA)和海藻酸钠(SA)为原料,过硫酸钾(KPS)为引发剂,在水溶液聚合法合成AM-AA共聚物/SA复合材料的基础上,添加淀粉和交联剂硝酸铝,采用造粒工艺制备了一种新型堵水剂AM-AA共聚物/SA复合材料小球(粒径约为3 mm),考察了SA用量、硝酸铝用量、淀粉用量和AA与AM单体的配比对堵水剂吸水性能的影响。实验结果表明,堵水剂的最佳制备条件为:1.4 mol/L AM、60 m L水、KPS用量1.0%(w)(基于单体AM和AA的质量)、SA用量6.0%(w)(基于AA,AM,SA的总质量)、硝酸铝用量0.6%(w)(基于复合材料的质量)、淀粉用量15.0%(w)(基于复合材料的质量)、n(AA)∶n(AM)=1.3、75℃、3 h。在该条件下制备的堵水剂吸水倍率最大,可达26.8 g/g,且凝胶强度好。

关键词：丙烯酰胺-丙烯酸共聚物/海藻酸钠复合材料堵水剂吸水性

Effect of Dachengqi Decoction on NF-κB p65 Expression in Lung of Rats with Partial Intestinal Obstruction and the Underlying Mechanism

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Journal of Huazhong University of Science and Technology(Medical Sciences) 2010年第2期30卷 217-221页

作者：杨胜兰沈霖金阳刘建国高洁嫦李道本 Department of Traditional Chinese Medicine Union HospitalTongji Medical CollegeHuazhong University of Science and Technology Department of Respiratory Diseases Union HospitalTongji Medical CollegeHuazhong University of Science and Technology

To investigate the effect of Dachengqi decoction on NF-κB p65 expression in lung of rats with partial intestinal obstruction and the underlying mechanism, 30 SD rats were randomly divided into three groups： sham-operation group, model group and Dachengqi decoction treatment group （Dachengqi group）, with 10 animals in each group. The models were made by partially ligating their large intestines outside the body. The pathological changes were analyzed by HE staining. The expression of NF-κB p65 in rats lung were measured by using real-time polymerase chain reaction and immunohistochemistry respectively. Moreover, the expression of caveolin-1 in rats lung was also measured to. Increased edema, interstitial thickening, hemorrhage, and infiltration of inflammatory cells were found in the model group. In contrast, this change was significantly reduced in Dachengqi group as compared with model group. In addition, the up-regulated caveolin-1 and NF-κB p65 were also suppressed by Dachengqi decoction in lung of rats with partial intestinal obstruction. We are led to concluded that the caveolin-l-NF-κB pathway plays an important role in the development of lung injury of rats with partial intestinal obstruction and Dachengqi decoction could down-regulate the expression of caveolin-1 and NF-κB p65 in lung of rats with partial intestinal obstruction.

关键词： Dachengqi decoction partial intestinal obstruction lung injury NF-κB p65 caveolin-1

抗真菌内切几丁质酶酶学性质及制备低聚壳寡糖功能分析

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食品科学 2024年第5期45卷 49-58页

作者：赵节昌王启源宋珂昕陈腾王峰杨杰高兆建徐州工程学院食品与生物工程学院江苏徐州221018 徐州奥卡姆食品有限公司江苏徐州221000 徐州鸿宇农业科技有限公司江苏徐州221000

为开发几丁质及壳聚糖生物转化活性寡聚糖并实现几丁质酶在食品防腐及生防方面的应用,从金色链霉菌(Streptomyces aureofaciens)XZ-Sa62中分离纯化几丁质酶(ChiA-Sa62),并研究其生物转化及抗菌功能。本实验采用Q-Sepharose Fast Flow、S... 详细信息

为开发几丁质及壳聚糖生物转化活性寡聚糖并实现几丁质酶在食品防腐及生防方面的应用,从金色链霉菌(Streptomyces aureofaciens)XZ-Sa62中分离纯化几丁质酶(ChiA-Sa62),并研究其生物转化及抗菌功能。本实验采用Q-Sepharose Fast Flow、Sephadex G-100层析和反相高效液相色谱纯化ChiA-Sa62,经纯化后ChiA-Sa62纯化倍数为41.3倍,比活力为1119.8 U/mg。并采用十二烷基硫酸钠-聚丙烯酰胺凝胶电泳和基质辅助激光解吸电离-飞行时间质谱测得ChiA-Sa62是分子质量为62.55 kDa的单亚基蛋白。ChiA-Sa62在50℃和pH 5.0的条件下,活性最高,并在60℃以下及pH 3.0~9.0范围内有良好稳定性。金属盐离子Ca^(2+)、Mn^(2+)、Mg^(2+)和Co^(2+)可激活酶活性。ChiA-Sa62对几丁质及脱乙酰度75%的壳聚糖具有专一内切水解活性,薄层色谱显示,水解产物分别为2~5个N-乙酰氨基葡萄糖单位的几丁寡糖和2~4个D-氨基葡萄糖单位的壳寡糖。ChiA-Sa62对底物胶体几丁质的米氏常数K_m和最大反应速率V_(max)值分别为2.75 mg/mL和64.52 U/mg。ChiA-Sa62可强烈抑制所试病原真菌菌丝生长;碘化丙啶染色显示,经ChiA-Sa62处理后的灰葡萄孢菌丝其细胞膜受到破坏。水解产物壳寡糖对致病性G^(-)菌(大肠杆菌和铜绿假单胞菌)和G~+菌(金黄色葡萄球菌和蜡样芽孢杆菌)有抑制作用,并且LIVE/DEAD染色显示壳寡糖可致使金黄色葡萄球菌死亡。本实验结果表明,Chi A-Sa62几丁质及壳聚糖在生物转化以及食品防腐及生物防治方面具有较大的应用潜力。

关键词：几丁质酶金色链霉菌酶学特性生物转化抗真菌活性

正肝化癥汤对原发性肝癌患者肝功能及AFP、CEA的影响

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光明中医 2021年第10期36卷 1644-1646页

作者：曹明满肖姬高洁嫦郑艳华刘月婵广州医科大学附属第二医院中医科广东广州510045

目的研究正肝化癥汤治疗原发性肝癌对患者肝功能及AFP、CEA的影响。方法选取收治的88例原发性肝癌患者,采取随机数字表法将其分为对照组(44例)和观察组(44例),对照组采取TACE治疗,观察组给予TACE联合正肝化癥汤治疗,2组治疗周期均为1个... 详细信息

目的研究正肝化癥汤治疗原发性肝癌对患者肝功能及AFP、CEA的影响。方法选取收治的88例原发性肝癌患者,采取随机数字表法将其分为对照组(44例)和观察组(44例),对照组采取TACE治疗,观察组给予TACE联合正肝化癥汤治疗,2组治疗周期均为1个月,对比2组患者的临床疗效,治疗前后肝功能及AFP、CEA水平。结果观察组的临床总有效率(97.73%)较对照组(75.00%)高;与治疗前比,治疗后2组患者的ALT、AST、AFP、CEA水平均下降,观察组较对照组低(均P<0.05)。结论正肝化癥汤治疗原发性肝癌可有效改善患者的临床症状,保护肝功能,降低血清AFP、CEA水平,有效抑制肿瘤生长转移。

关键词：正肝化癥汤臌胀原发性肝癌肝功能中医药疗法

抵当汤对糖尿病兔腹主动脉球囊损伤后血管重构的研究

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新中医 2017年第8期49卷 11-15页

作者：曹明满吕雄陈婧郑艳华庞如菲高洁嫦肖姬广州医科大学附属第二医院(番禺院区中医科) 广东广州511447 广东省第二中医院广东广州510095

目的 :探讨抵当汤对糖尿病兔腹主动脉球囊损伤后血管重构的作用及机制。方法 :首先建立糖尿病兔模型,分为假手术组、模型组、抵当汤低剂量组、抵当汤高剂量组、Y-27632组,除假手术组外,其他各组兔接受球囊损伤手术,建立糖尿病实验兔腹... 详细信息

目的 :探讨抵当汤对糖尿病兔腹主动脉球囊损伤后血管重构的作用及机制。方法 :首先建立糖尿病兔模型,分为假手术组、模型组、抵当汤低剂量组、抵当汤高剂量组、Y-27632组,除假手术组外,其他各组兔接受球囊损伤手术,建立糖尿病实验兔腹主动脉球囊损伤模型。模型组接受生理盐水胃管注入;Y-27632组接受Y-27632胃管注入,给药剂量为70 mg/(kg·d);抵当汤低剂量组、抵当汤高剂量组分别给予8.1 g/(kg·d)、16.2 g/(kg·d)的抵当汤胃管注射。术后通过血管影像学、病理学方法观察抵当汤对糖尿病实验兔腹主动脉球囊损伤后血管内径、内膜、中膜、血流速度等的影响。结果:与假手术组比较,模型组动脉内径和血流速度均明显降低,管腔面积和内膜包绕面积显著减少,内膜面积和中膜面积显著增加,差异均有统计学意义(P<0.05,P<0.01),说明以动脉内膜增殖及管腔狭窄为特征的糖尿病实验兔腹主动脉球囊损伤后动脉损伤模型造模成功。与模型组比较,Y-27632组的动脉内径显著升高,抵当汤高剂量组和抵当汤低剂量组的动脉内径和血流速度均显著升高,Y-27632组、抵当汤低剂量组、抵当汤高剂量组的中膜面积显著降低,抵当汤低剂量组和抵当汤高剂量组的内膜包绕面积均增加,差异均有统计学意义(P<0.05,P<0.01)。与Y-27632组比较,抵当汤高剂量组血流速度显著升高,内膜面积和中膜面积显著降低,内膜包绕面积显著增加,差异均有统计学意义(P<0.05)。与抵当汤低剂量组比较,抵当汤高剂量组血流速度显著升高,内膜面积和中膜面积显著降低,差异均有统计学意义(P<0.05,P<0.01)。结论:抵当汤可以改善糖尿病实验兔腹主动脉球囊损伤后的血管重构。

关键词：糖尿病血管病变抵当汤中药疗法血管重构疾病模型新西兰大耳白兔