The Ru-catalyzed carbonylation of alkenes with CO_(2)as a C1 surrogate and imidazole chlorides as the promotor is investigated by a combination of computational and experimental study.The conversion rate of CO_(2)to C...The Ru-catalyzed carbonylation of alkenes with CO_(2)as a C1 surrogate and imidazole chlorides as the promotor is investigated by a combination of computational and experimental study.The conversion rate of CO_(2)to CO is positively correlated with the efficiency of both hydroesterification and hydroformylation,which is found facilitated in the presence of chloride additives with a decreasing order of BmimCl~B3MimCl>BmmimCl~LiCl.Taking the hydroesterification with MeOH as a representative example,BmimCl bearing C-H functionality at the C^(2)site of the cation assists the reduction of CO_(2)to CO as a hydrogen donor medium,with the anion and cation acting in a synergistic fashion.Subsequent insertion of CO_(2)into the formed Ru-H bond with the assistance of chloride anion produces the Ru-COOH species,which ultimately accelerates the activation of CO_(2).展开更多
目的研究磷酸西格列汀联合氯沙坦钾对糖尿病肾病患者炎症因子、纤维化指标及血管内皮因子的影响。方法选取2016年3月-2017年6月东部战区总医院确诊糖尿病肾病患者80例,依据随机数字表法分为观察组和对照组,每组40例。所有患者均予氯沙...目的研究磷酸西格列汀联合氯沙坦钾对糖尿病肾病患者炎症因子、纤维化指标及血管内皮因子的影响。方法选取2016年3月-2017年6月东部战区总医院确诊糖尿病肾病患者80例,依据随机数字表法分为观察组和对照组,每组40例。所有患者均予氯沙坦钾与二甲双胍缓释片治疗,4周后观察组患者予磷酸西格列汀100 mg/d,1次/d。治疗12周后观察比较两组患者血糖和肾功能相关指标的变化情况;比较两组治疗前后炎症因子、纤维化相关指标及血管内皮相关因子水平变化,记录两组不良反应的发生情况。结果治疗前两组患者血糖差异无统计学意义(P>0.05);治疗后两组空腹血糖(FPG)、餐后2 h血糖(2 h PG)和糖化血红蛋白(HbA1c)降低,观察组低于对照组(P<0.05);治疗后两组微量白蛋白尿(mAlb)、尿蛋白肌酐比值和血清胱抑素C浓度降低,观察组低于对照组(P<0.05);治疗后两组白细胞介素-6(IL-6)、肿瘤坏死因子-α(TNF-α)和C反应蛋白(CRP)水平降低,观察组低于对照组(P<0.05);治疗后两组血清基质金属蛋白酶-9(MMP-9)、层黏蛋白(LN)、透明质酸(HA)、Ⅲ型前胶原(PCⅢ)和Ⅳ型胶原(ⅣC)水平降低,对照组低于观察组(P<0.05);治疗后两组内皮素(ET)水平降低,观察组低于对照组(P<0.05);两组一氧化氮NO水平治疗后较治疗前升高,观察组高于对照组(P<0.05);两组不良反应发生率比较差异无统计学意义(P>0.05)。结论磷酸西格列汀联合氯沙坦钾治疗糖尿病肾病可抑制机体炎症状态,延缓纤维化进程,改善血管内皮舒缩功能,对肾功能起到保护作用。展开更多
Members of Veratrum are perennial herbs widely used in traditional Chinese medicine to induce vomiting,resolve blood stasis and relieve pain.However,the intrageneric classification and phylogenetic relationships withi...Members of Veratrum are perennial herbs widely used in traditional Chinese medicine to induce vomiting,resolve blood stasis and relieve pain.However,the intrageneric classification and phylogenetic relationships within Veratrum have long been controversial due to the complexity of morphological variations and lack of high-resolution molecular markers.In this study,we reevaluated the infrageneric relationships with the genus Veratrum using complete chloroplast genome sequence data.Herein,the complete cp genomes of ten species of Veratrum were newly sequenced and characterized.The complete cp genomes of ten species of Veratrum had the typical quadripartite structure,ranging from 151,597 bp to 153,711 bp in size and comprising a total of 135 genes.The structure of Veratrum cp genomes(i.e.,gene order,content,and genome components)was highly similar across species.The number of simple sequence repeats(SSRs)ranged from 63 to 7&and of long repeats ranged from 31 to 35.Eight highly divergent regions(ndhF,psbC-psbZ,psbK-psbl,rpoB-tmCjGCA,tmK_UUU-tmQ_UUG,tmS_GCU-tmG_UCC,tmT_UGU-tmL_UAA and ycfl)were identified and are potentially useful for the DNA barcoding of Veratrum.Phylogenetic analysis among 29 taxa based on cp genomes,total genes,protein-coding genes and intergenic regions strongly supported the monophyly of Veratrum.The circumscription and relationships of the infrageneric taxa of Veratrum were well-presented with great resolution.These results will facilitate the identification,taxonomy,and utilization of Veratrum plants as well as the evolutionary studies of Melanthiaceae.展开更多
Electrocatalytic reduction of CO_(2)(CO_(2)RR)to multi-electron(>2e–)products provides a green and sustainable route for producing fuels and chemicals.Introducing the second metal element is a feasible strategy fo...Electrocatalytic reduction of CO_(2)(CO_(2)RR)to multi-electron(>2e–)products provides a green and sustainable route for producing fuels and chemicals.Introducing the second metal element is a feasible strategy for"managing"the key intermediate on Cu-based materials to further improve the CO_(2)RR catalytic performance.In this work,palladium,which promises the generation of CO,was introduced into the poly(ionic liquid)-based copper hybrid(Cu@PIL)to construct a novel Cu-Pd bimetallic electrocatalyst(Cu@PIL@Pd).Remarkably,with a small dosage of palladium(2.0 mol%compared with Cu),a high faradaic efficiency(FE)for C_(2+)products(68.7%)was achieved at–1.01 V(with respect to the reversible hydrogen electrode(RHE),the same below)with a high partial current density of 178.3 mA cm^(-2).Meanwhile,high selectivity towards CH4(FE=42.5%)and corresponding partial current density of 172.8 mA cm^(-2)were obtained on the same catalyst at–1.24 V,signifying a significant potential-dependent selectivity.Mechanistic studies reveal that both copper and palladium oxides are reduced to metallic states during the CO_(2)RR.The presence of the adjoint copper phase and the highly dispersed electrostatic layer promote the generation of CO on the palladium components(both the PdO_(2)phase and the Pd(II)site).Besides,the local CO^(*)was enriched by the significant diffusion resistance of CO in the PIL layer.The spillover of CO^(*)from Pd sites to the adjoint Cu sites,accompanied by the increased local concentration of CO^(*)around Cu sites,accounted for the observed good CO_(2)RR catalytic performance,especially the high C_(2+)product selectivity.展开更多
基金Financial support from National Natural Science Foundation of China (22078336, U1662133, 21773158, 22008238)Innovation Academy for Green Manufacture, CAS (IAGM2020C13) is gratefully acknowledged
文摘The Ru-catalyzed carbonylation of alkenes with CO_(2)as a C1 surrogate and imidazole chlorides as the promotor is investigated by a combination of computational and experimental study.The conversion rate of CO_(2)to CO is positively correlated with the efficiency of both hydroesterification and hydroformylation,which is found facilitated in the presence of chloride additives with a decreasing order of BmimCl~B3MimCl>BmmimCl~LiCl.Taking the hydroesterification with MeOH as a representative example,BmimCl bearing C-H functionality at the C^(2)site of the cation assists the reduction of CO_(2)to CO as a hydrogen donor medium,with the anion and cation acting in a synergistic fashion.Subsequent insertion of CO_(2)into the formed Ru-H bond with the assistance of chloride anion produces the Ru-COOH species,which ultimately accelerates the activation of CO_(2).
文摘目的研究磷酸西格列汀联合氯沙坦钾对糖尿病肾病患者炎症因子、纤维化指标及血管内皮因子的影响。方法选取2016年3月-2017年6月东部战区总医院确诊糖尿病肾病患者80例,依据随机数字表法分为观察组和对照组,每组40例。所有患者均予氯沙坦钾与二甲双胍缓释片治疗,4周后观察组患者予磷酸西格列汀100 mg/d,1次/d。治疗12周后观察比较两组患者血糖和肾功能相关指标的变化情况;比较两组治疗前后炎症因子、纤维化相关指标及血管内皮相关因子水平变化,记录两组不良反应的发生情况。结果治疗前两组患者血糖差异无统计学意义(P>0.05);治疗后两组空腹血糖(FPG)、餐后2 h血糖(2 h PG)和糖化血红蛋白(HbA1c)降低,观察组低于对照组(P<0.05);治疗后两组微量白蛋白尿(mAlb)、尿蛋白肌酐比值和血清胱抑素C浓度降低,观察组低于对照组(P<0.05);治疗后两组白细胞介素-6(IL-6)、肿瘤坏死因子-α(TNF-α)和C反应蛋白(CRP)水平降低,观察组低于对照组(P<0.05);治疗后两组血清基质金属蛋白酶-9(MMP-9)、层黏蛋白(LN)、透明质酸(HA)、Ⅲ型前胶原(PCⅢ)和Ⅳ型胶原(ⅣC)水平降低,对照组低于观察组(P<0.05);治疗后两组内皮素(ET)水平降低,观察组低于对照组(P<0.05);两组一氧化氮NO水平治疗后较治疗前升高,观察组高于对照组(P<0.05);两组不良反应发生率比较差异无统计学意义(P>0.05)。结论磷酸西格列汀联合氯沙坦钾治疗糖尿病肾病可抑制机体炎症状态,延缓纤维化进程,改善血管内皮舒缩功能,对肾功能起到保护作用。
文摘Members of Veratrum are perennial herbs widely used in traditional Chinese medicine to induce vomiting,resolve blood stasis and relieve pain.However,the intrageneric classification and phylogenetic relationships within Veratrum have long been controversial due to the complexity of morphological variations and lack of high-resolution molecular markers.In this study,we reevaluated the infrageneric relationships with the genus Veratrum using complete chloroplast genome sequence data.Herein,the complete cp genomes of ten species of Veratrum were newly sequenced and characterized.The complete cp genomes of ten species of Veratrum had the typical quadripartite structure,ranging from 151,597 bp to 153,711 bp in size and comprising a total of 135 genes.The structure of Veratrum cp genomes(i.e.,gene order,content,and genome components)was highly similar across species.The number of simple sequence repeats(SSRs)ranged from 63 to 7&and of long repeats ranged from 31 to 35.Eight highly divergent regions(ndhF,psbC-psbZ,psbK-psbl,rpoB-tmCjGCA,tmK_UUU-tmQ_UUG,tmS_GCU-tmG_UCC,tmT_UGU-tmL_UAA and ycfl)were identified and are potentially useful for the DNA barcoding of Veratrum.Phylogenetic analysis among 29 taxa based on cp genomes,total genes,protein-coding genes and intergenic regions strongly supported the monophyly of Veratrum.The circumscription and relationships of the infrageneric taxa of Veratrum were well-presented with great resolution.These results will facilitate the identification,taxonomy,and utilization of Veratrum plants as well as the evolutionary studies of Melanthiaceae.
基金Key Research Program of Frontier Sciences,CAS(ZDBS-LY-JSC022)Excellent Young Scientists Fund(22022815)+1 种基金National Natural Science Foundation of China(U1704251 and 21776291)Zhengzhou High Level Talent Certificate(20180200052)is gratefully acknowledged.
文摘Electrocatalytic reduction of CO_(2)(CO_(2)RR)to multi-electron(>2e–)products provides a green and sustainable route for producing fuels and chemicals.Introducing the second metal element is a feasible strategy for"managing"the key intermediate on Cu-based materials to further improve the CO_(2)RR catalytic performance.In this work,palladium,which promises the generation of CO,was introduced into the poly(ionic liquid)-based copper hybrid(Cu@PIL)to construct a novel Cu-Pd bimetallic electrocatalyst(Cu@PIL@Pd).Remarkably,with a small dosage of palladium(2.0 mol%compared with Cu),a high faradaic efficiency(FE)for C_(2+)products(68.7%)was achieved at–1.01 V(with respect to the reversible hydrogen electrode(RHE),the same below)with a high partial current density of 178.3 mA cm^(-2).Meanwhile,high selectivity towards CH4(FE=42.5%)and corresponding partial current density of 172.8 mA cm^(-2)were obtained on the same catalyst at–1.24 V,signifying a significant potential-dependent selectivity.Mechanistic studies reveal that both copper and palladium oxides are reduced to metallic states during the CO_(2)RR.The presence of the adjoint copper phase and the highly dispersed electrostatic layer promote the generation of CO on the palladium components(both the PdO_(2)phase and the Pd(II)site).Besides,the local CO^(*)was enriched by the significant diffusion resistance of CO in the PIL layer.The spillover of CO^(*)from Pd sites to the adjoint Cu sites,accompanied by the increased local concentration of CO^(*)around Cu sites,accounted for the observed good CO_(2)RR catalytic performance,especially the high C_(2+)product selectivity.
