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一维g-C_(3)N_(4)/二维Ti_(3)C_(2)Tx界面调制促进光催化CO_(2)还原活性与选择性
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作者 钟蕤羽 梁玉洁 +2 位作者 黄菲 梁诗诺 刘升卫 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2023年第10期109-122,共14页
碳中和是实现绿色可持续发展重要途径之一,以半导体光催化CO_(2)还原.反应(CO_(2)RR)为核心的人工光合成技术极具发展前景.石墨相氮化碳(g-C_(3)N_(4))作为一种二维层状光催化剂,化学性质稳定,且满足CO_(2)RR的热力学要求,但传统的g-C_(... 碳中和是实现绿色可持续发展重要途径之一,以半导体光催化CO_(2)还原.反应(CO_(2)RR)为核心的人工光合成技术极具发展前景.石墨相氮化碳(g-C_(3)N_(4))作为一种二维层状光催化剂,化学性质稳定,且满足CO_(2)RR的热力学要求,但传统的g-C_(3)N_(4)光催化活性和选择性较低,这主要归因于高的电荷复合几率和低的光电子利用效率.采用二维碳化钛(Ti_(3)C_(2)Tx)等碳基助催化剂作为电子受体,促进光生载流子的快速分离与转移,成为提高g-C_(3)N_(4)光催化CO_(2)RR效率的有效手段.然而,g-C_(3)N_(4)光催化剂与Ti_(3)C_(2)Tx助催化剂多数以2D/2D构型界面耦合,受限于二者界面弱的范德华相互作用、高的界面静电势垒和缓慢的界面电荷转移速率,2D/2D g-C_(3)N_(4)/Ti_(3)C_(2)Tx肖特基结光催化CO_(2)RR活性与选择性仍普遍欠佳.针对该问题,本文采用熔盐法制备了沿c轴方向生长的1D高结晶g-C_(3)N_(4)纳米棒(CCN),并通过冷冻干燥辅助界面耦合的方法将其组装到2D Ti_(3)C_(2)Tx基底上,在冷冻干燥条件下,CCN边缘的NHx与MXene表面-O/-OH基团会形成更强的界面氢键耦合作用,最终构筑具有独特界面氢键作用的1D/2D肖特基结光催化剂(记作1D/2D TC/CCN-FD).扫描电镜和透射电镜结果证明了复合材料的成功制备.X射线光电子能谱和密度泛函理论(DFT)计算结果证明了界面电荷的定向转移.瞬态光电流、Nyquist曲线、荧光光谱和DFT计算结果表明,由于g-C_(3)N_(4)纳米棒光催化剂沿π共轭平面的电荷传输势垒远低于以范德华相互连接的g-C_(3)N_(4)层间的电荷传输势垒,1D/2D构型界面耦合可以降低界面电荷转移能垒,加快界面电荷转移速率.气相色谱结果表明,优化组成结构得到的1D/2D TC/CCN-FD复合光催化剂表现出较好的光催化CO_(2)还原效率(2.13μmol^(-1)h^(-1)),分别是1D CCN和2D传统氮化碳的5.6和8.9倍.同时,2D Ti_(3)C_(2)Tx助催化剂上富集的更高密度的光电子,促使多电子还原产物(CH_(4))的选择性显著提高到60%以上(产率为1.4μmol g-1h^(-1)).原位漫反射红外傅里叶变换光谱和同位素标定结果进一步明确了CO_(2)RR反应路径和反应机理.综上所述,本文揭示了界面晶体取向匹配与界面强耦合作用对促进高效界面光电子定向迁移具有重要协同作用,为未来开发高性能异质结光催化剂提供新思路. 展开更多
关键词 碳化钛 高结晶氮化碳 一维/二维 光催化二氧化碳还原 助催化剂
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Neck observation versus elective neck dissection in management of clinical T1/2N0 oral squamous cell carcinoma: a retrospective study of 232 patients 被引量:2
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作者 Xiangqi Liu Xiaomei Lao +4 位作者 Lizhong liang Sien Zhang Kan Li Guiqing Liao yujie liang 《Chinese Journal of Cancer Research》 SCIE CAS CSCD 2017年第3期179-188,共10页
Objective: The management of early-stage(cT1/2N0) oral squamous cell carcinoma(OSCC) remains a controversial issue. The aim of this study was to compare the clinical outcomes of neck observation(OBS) and elective neck... Objective: The management of early-stage(cT1/2N0) oral squamous cell carcinoma(OSCC) remains a controversial issue. The aim of this study was to compare the clinical outcomes of neck observation(OBS) and elective neck dissection(END) in treating patients with cT1/2N0 OSCC.Methods: A total of 232 patients with cT1/2N0 OSCC were included in this retrospective study. Of these patients, 181 were treated with END and 51 with OBS. The survival curves of 5-year overall survival(OS), diseasespecific survival(DSS), and recurrence-free survival(RFS) rates were plotted using the Kaplan-Meier method for each group, and compared using the Log-rank test.Results: There was no significant difference in 5-year OS and DSS rates between END and OBS groups(OS:89.0% vs. 88.2%, P=0.906; DSS: 92.3% vs. 92.2%, P=0.998). However, the END group had a higher 5-year RFS rate than the OBS group(90.1% vs. 76.5%, P=0.009). Patients with occult metastases in OBS group(7/51) had similar 5-year OS rate(57.1% vs. 64.1%, P=0.839) and DSS rate(71.4% vs. 74.4%, P=0.982) to those in END group(39/181). In the regional recurrence patients, the 5-year OS rate(57.1% vs. 11.1%, P=0.011) and DSS rate(71.4% vs. 22.2%, P=0.022) in OBS group(7/51) were higher than those in END group(9/181).Conclusions: The results indicated that OBS policy could obtain the same 5-year OS and DSS as END. Under close follow-up, OBS policy may be an available treatment option for patients with clinical T1/2N0 OSCC. 展开更多
关键词 Lymphatic metastasis neck dissection neck observation oral squamous cell carcinoma SURVIVAL
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Ex vivo cartilage explant model for the evaluation of chondrocyte-targeted exosomes
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作者 KAN OUYANG MEIQUAN XU +8 位作者 yujie liang XIAO XU LIMEI XU CAINING WEN ZHUAN QIN YIXIN XIE HUAWEI ZHANG LI DUAN DAPING WANG 《BIOCELL》 SCIE 2022年第6期1521-1526,共6页
There is no efficient tracking system available for the therapeutic molecules delivered to cartilage.The dense matrix covering the cartilage surface is the main biological barrier that the therapeutic molecules must o... There is no efficient tracking system available for the therapeutic molecules delivered to cartilage.The dense matrix covering the cartilage surface is the main biological barrier that the therapeutic molecules must overcome.In this study,we aimed to establish a system that can dynamically and effectively track the therapeutic molecules delivered to cartilage.To this aim,we adopted bovine and human cartilage explants as ex vivo models for chondrocyte-targeted exosome dispersion.The efficiency of drug delivery was evaluated using frozen sections.The results of this study showed that the penetration and distribution of chondrocyte-targeted exosomes in cartilage explants can be tracked dynamically.Thus,ex vivo cartilage explants provide an effective and economic system to evaluate therapeutic drugs encapsulated in chondrocyte-targeted exosomes in preclinical studies. 展开更多
关键词 Cartilage explants EXOSOMES Targeted delivery
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Hierarchical three-dimensional flower-like Co3O4 archi- tectures with a mesocrystal structure as high capacity anode materials for long-lived lithium-ion batteries 被引量:6
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作者 Wenqiang Cao Wenzhong Wang +4 位作者 Honglong Shi Jun Wang Maosheng Cao yujie liang Min Zhu 《Nano Research》 SCIE EI CAS CSCD 2018年第3期1437-1446,共10页
关键词 锂离子电池 CO3O4 体系结构 能力 阳极材料 长寿 三维 离子存储
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Copper-Catalyzed Asymmetric Hydroamination:A Unified Strategy for the Synthesis of Chiralβ-Amino Acid and Its Derivatives 被引量:1
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作者 Ge Zhang yujie liang +4 位作者 Tao Qin Tao Xiong Shuyu Liu Wei Guan Qian Zhang 《CCS Chemistry》 CAS 2021年第7期1737-1745,共9页
Catalytic asymmetric aza-Michael represents one of the most convenient and atom-economical approaches for the rapid construction of biologically active chiralβ-amino acid frameworks.However,the direct enantioselectiv... Catalytic asymmetric aza-Michael represents one of the most convenient and atom-economical approaches for the rapid construction of biologically active chiralβ-amino acid frameworks.However,the direct enantioselective addition of nitrogen-based nucleophiles to intrinsically low reactivity ofα,β-unsaturated carboxylic acid,ester,and amide,as well as simpleα,β-unsaturated nitrile,remains a long-standing challenge. 展开更多
关键词 asymmetric catalysis reversal hydroamination chiralβ-amino acid and its derivatives copper catalysis Michael acceptors
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CsOH catalyzed aerobic oxidative synthesis of p-quinols from multi-alkyl phenols under mild conditions
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作者 Yu-Feng liang Kai Wu +4 位作者 Zhiqing Liu Xiaoyang Wang yujie liang Chenjiang Liu Ning Jiao 《Science China Chemistry》 SCIE EI CAS CSCD 2015年第8期1334-1339,共6页
p-Quinols are ubiquitous structural motifs of various natural products and pharmaceutical compounds,and versatile building blocks in synthetic chemistry.The reported methods for the synthesis of p-quinol require stoic... p-Quinols are ubiquitous structural motifs of various natural products and pharmaceutical compounds,and versatile building blocks in synthetic chemistry.The reported methods for the synthesis of p-quinol require stoichiometric amounts of oxidants.Molecular oxygen is considered as an ideal oxidant due to its natural,inexpensive,and environmentally friendly characteristics.During the ongoing research of C–H bond hydroxylation,we found that multi-alkyl phenols could react with molecular oxygen under mild conditions.Herein,we describe an efficient oxidative de-aromatization of multi-alkyl phenols to p-quinols.1 atm of molecular oxygen was used as the oxidant.Many multi-alkyl phenols could react smoothly at room temperature.Isotopic labeling experiment was also performed,and the result proved that the oxygen atom in the produced hydroxyl group is from molecular oxygen. 展开更多
关键词 烷基酚类化合物 催化氧化合成 氢氧化铯 同位素标记 分子氧 氧化剂 天然产物 合成化学
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Copper-catalyzed enantioselective cyanation of benzylic C–H bonds via radical relay
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作者 yujie liang Ning Jiao 《Science China Chemistry》 SCIE EI CAS CSCD 2017年第1期105-106,共2页
Direct methods that enable stereoselective functionalization of C(sp^3)–H bonds could facilitate efficient preparation of therapeutics and agrochemicals,and shall have a major effect on the discovery and development ... Direct methods that enable stereoselective functionalization of C(sp^3)–H bonds could facilitate efficient preparation of therapeutics and agrochemicals,and shall have a major effect on the discovery and development of new pharmaceuticals.Although the transformations through C(sp^2)–H bond cleavage have been significantly developed in the past decades,the direct C(sp^3)–H functionalization,especially the asymmetric transformation is still a big challenge.Demon- 展开更多
关键词 不对称 铜催化 氰化 中继 苄基 高效制备 治疗药物 药物发现
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Dynamic changes of wound-related miRNAs after application of autologous platelet-rich gel in diabetic wounds
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作者 Yan Li yujie liang +2 位作者 Yunyi Gao Dawei Chen Xingwu Ran 《Chinese Medical Journal》 SCIE CAS CSCD 2022年第21期2644-2646,共3页
To the Editor:Diabetic chronic cutaneous ulcers(DCUs)are among the most common and serious complications of diabetes mellitus.Diabetic foot ulcers are the most common type of DCU and are now considered a global epidem... To the Editor:Diabetic chronic cutaneous ulcers(DCUs)are among the most common and serious complications of diabetes mellitus.Diabetic foot ulcers are the most common type of DCU and are now considered a global epidemic.[1]The clinical prevention and treatment of DCUs are critical and have remained challenging for clinicians.With the exploration of topical treatment methods,autologous platelet-rich gel(APG)is regarded as an adjuvant therapy to promote wound healing,and it has been widely used for wound repair.[2]Some microRNAs that play a critical role in the whole wound healing process have been found in wound tissues,which we call wound-related miRNAs(wr-miRNAs).However,few studies have explored the dynamic changes of wr-miRNAs during APG treatment.Our study aimed to evaluate the efficacy of APG in treating diabetic wounds and explore the dynamic changes of wr-miRNAs during wound healing. 展开更多
关键词 PREVENTION TREATMENT MIRNAS
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Efficient Pd-Catalyzed C-H Oxidative Bromination of Arenes with Dimethyl Sulfoxide and Hydrobromic Acid
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作者 Yizhi Yuan yujie liang +2 位作者 Shihui Shi Yu-Feng liang Ning Jiao 《Chinese Journal of Chemistry》 SCIE CAS CSCD 2020年第11期1245-1251,共7页
of main observation and conclusion We have developed an efficient Pd-catalyzed directed C-H bromination protocol,in which dimethyl sulfoxide(DMSO)is employed as oxidant with hydrobromic add aqueous solution(HBr(aq))as... of main observation and conclusion We have developed an efficient Pd-catalyzed directed C-H bromination protocol,in which dimethyl sulfoxide(DMSO)is employed as oxidant with hydrobromic add aqueous solution(HBr(aq))as bromide source.The DMSO/HBr(aq)system,which is novelly and efficiently utilized in transition-metal catalyzed C-H activation,illustrates its practicability by the operational simplicity,inexpensive and readily available starting materials,and high bromide-atom economy. 展开更多
关键词 CATALYZED BROMIDE SIMPLICITY
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Nitromethane-Enabled Fluorination of Styrenes and Arenes
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作者 Weijin Wang Tongyu Huo +5 位作者 Xinyi Zhao Qixue Qin yujie liang Song Song Guosheng Liu Ning Jiao 《CCS Chemistry》 CAS 2020年第6期566-575,共10页
The electrophilic fluorination of unsaturated compounds provides a reliable approach to the generation of organofluorides,which are used widely in agrochemicals,pharmaceuticals,and other materials.Numerous active elec... The electrophilic fluorination of unsaturated compounds provides a reliable approach to the generation of organofluorides,which are used widely in agrochemicals,pharmaceuticals,and other materials.Numerous active electrophilic fluorine reagents,such as the fluorine molecule(F_(2))or xenon difluoride(XeF_(2)),have been applied in fluorination.However,these reagents suffer from their hazardous,toxic,corrosive,and poor selective properties,and the relatively weak electrophilicity of Selectfluor or N-fluorobenzenesulfonimide(NFSI)usually limits their broad applications.Herein,we disclose nitromethane(MeNO_(2))as an efficient activator of Selectfluor and NFSI,as well as a stabilizer of carbocations.Therefore,the fluoro-azidation,fluoroamination,fluoroesterification of styrenes,and C–H fluorination of(hetero)arenes were well realized just by the facilitation of MeNO_(2).The mild reaction conditions and practicability made our current method a versatile protocol for accessing organofluorides. 展开更多
关键词 fluoroazidation fluoroamination fluoroesterification electrophilic fluorination NITROMETHANE
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