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单原子修饰原子簇的多配位Cu基催化剂上CO_(2)高选择性电还原CO的研究
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作者 王超琛 葛旺鑫 +6 位作者 唐雷 齐宴宾 董磊 江宏亮 沈建华 朱以华 李春忠 《Chinese Journal of Catalysis》 SCIE CAS CSCD 2024年第4期324-333,共10页
随着可再生能源发电成本的持续下降和电催化技术的迅猛发展,人们开始重新审视能源燃料和化学品的生产方式.近年来,H2O和CO_(2)等小分子的电催化转化反应已成为研究热点.特别是,CO_(2)还原反应(CO_(2)RR)作为将CO_(2)电化学还原为高附加... 随着可再生能源发电成本的持续下降和电催化技术的迅猛发展,人们开始重新审视能源燃料和化学品的生产方式.近年来,H2O和CO_(2)等小分子的电催化转化反应已成为研究热点.特别是,CO_(2)还原反应(CO_(2)RR)作为将CO_(2)电化学还原为高附加值产品的一项变革性的技术,备受关注.在CO_(2)RR的众多产物中,CO具有重要的地位,它可以通过费托合成工艺直接用于合成醇、醛、酮、酸及烃等化工产品.然而,将CO_(2)电催化转化为CO在整体效率方面仍面临诸多挑战.因此,设计并制备高效、经济且耐用的电催化剂已成为CO_(2)RR领域发展的研究重点.本文采用简单的配体辅助负载策略制备了铜单原子修饰的铜原子簇催化剂(Cu SA/ACs).球差校正的高角度环形暗场扫描透射电子显微镜结果表明,铜以单原子和原子簇的形式存在.采用X射线吸收精细结构谱和X射线光电子能谱(XPS)分析了铜原子的电子和配位结构,证明了Cu-N键和Cu-Cu键的存在.电化学性能测试表明,与铜单原子催化剂(Cu SACs)相比,Cu SA/ACs催化剂展现了较好的CO_(2)RR性能,其CO的转化法拉第效率从27.15%提高到98.94%,电流密度是Cu SACs的3.6倍.此外,将该催化剂组装成流动电解池,在600 mA cm-2的高电流密度下,CO选择性达到93.06%,阴极的最高能量效率达61.9%,优于大多数CO_(2)还原制备CO的催化剂.为了明确铜单原子组分引入对铜原子簇性能提升的原因,通过电化学原位红外光谱研究催化剂在服役条件下的表面物种吸附.结果表明,Cu SACs催化剂的单原子活性中心在CO_(2)RR过程中受到H2析出反应的困扰,活性中心表面的吸附物种主要为H2O而不是CO_(2),从而导致CO_(2)还原性能较差;在Cu SA/ACs催化剂表面,其活性中心由单原子和原子簇协同组成,CO_(2)主要吸附在原子簇上,单原子和原子簇协同作用促进了H2O的解离过程,为CO_(2)质子化提供丰富的活性氢,进一步加快CO_(2)RR的反应动力学.密度泛函计算和差分电荷密度分析结果表明,单原子的引入优化了原子簇的局域电子结构,诱导d带中心靠近费米能级,从而优化了*COOH中间体的形成能和CO的脱附过程.综上,本文通过合理的活性位点设计实现了多位点的耦合协同,提升了铜基催化剂对于CO_(2)RR的催化活性,优化了铜基催化剂上CO_(2)到CO的选择性,通过机理研究加深了对铜基催化剂上CO_(2)转化模式的认识,为设计高效催化剂提供新思路. 展开更多
关键词 二氧化碳还原 活性位点协同作用 单原子 原子簇 电催化
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New insights into effects of Kaixin Powder on depression via lipid metabolism related adiponectin signaling pathway 被引量:2
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作者 Wenshan Yang Hong Yin +5 位作者 Yichen wang Yuanbo wang Xia Li chaochen wang Ping Liu Yuan Hu 《Chinese Herbal Medicines》 CAS 2023年第2期240-250,共11页
Objective:To clarify the anti-depressive potential mechanisms of Kaixin Powder(KP),a drug that helps to prevent and treat depression and other mentaldiseases,from genome-wide transcriptome profiling.Methods:Transcript... Objective:To clarify the anti-depressive potential mechanisms of Kaixin Powder(KP),a drug that helps to prevent and treat depression and other mentaldiseases,from genome-wide transcriptome profiling.Methods:Transcriptome and KEGG pathway analysis were conducted on the hippocampus of depressed rats,then the differentially expressed genes were validated and serum concentration of lipid parameters were identified by enzymatic assays.Furthermore,high-fat diets induced depression-like behaviors in Syrian golden hamsters were conducted to verify the predicted molecular mechanisms acquired from the transcriptome analysis.Results:Transcriptome results revealed that the 24 differentially expressed genes(DEGs)in chronic mild stress(CMS)rats could be reversed after two weeks of KP treatment.The mechanisms of KP in treating depression firstly involved the regulation of several pathology modules,including lipid metabolism,synapse function and inflammation.KP could regulate imbalances of lipid homeostasis in high-fat diet induced depressive symptoms.Furthermore,it was validated that cholesterol metabolism dysfunction can be ameliorated by KP,which was correlated with upregulation of the AdipoR1-BDNF(brainderived neurotrophic factor)co-regulatory pathway.Conclusion:Taken together,our results demonstrated that KP not only alleviates depression via traditional mental illness targets,but it may also simulates the cholesterol metabolism and adiponectin signaling with multi-target characteristics. 展开更多
关键词 ADIPONECTIN cholesterol homeostasis DEPRESSION high-fat diet Kaixin Powder transcriptome analysis
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