Urea generation through electrochemical CO_(2) and NO_(3)~-co-reduction reaction(CO_(2)NO_(3)RR)is still limited by either the low selectivity or yield rate of urea.Herein,we report copper carbonate hydroxide(Cu_2(OH)...Urea generation through electrochemical CO_(2) and NO_(3)~-co-reduction reaction(CO_(2)NO_(3)RR)is still limited by either the low selectivity or yield rate of urea.Herein,we report copper carbonate hydroxide(Cu_2(OH)_2CO_(3))as an efficient CO_(2)NO_(3)RR electrocatalyst with an impressive urea Faradaic efficiency of45.2%±2.1%and a high yield rate of 1564.5±145.2μg h~(-1)mg_(cat)~(-1).More importantly,H_(2) evolution is fully inhibited on this electrocatalyst over a wide potential range between-0.3 and-0.8 V versus reversible hydrogen electrode.Our thermodynamic simulation reveals that the first C-N coupling follows a unique pathway on Cu_2(OH)_2CO_(3) by combining the two intermediates,~*COOH and~*NHO.This work demonstrates that high selectivity and yield rate of urea can be simultaneously achieved on simple Cu-based electrocatalysts in CO_(2)NO_(3)RR,and provide guidance for rational design of more advanced catalysts.展开更多
Electrochemical C-C and C-N coupling reactions with the conversion of abundant and inexpensive small molecules,such as CO_(2) and nitrogencontaining species,are considered a promising route for increasing the value of...Electrochemical C-C and C-N coupling reactions with the conversion of abundant and inexpensive small molecules,such as CO_(2) and nitrogencontaining species,are considered a promising route for increasing the value of CO_(2) reduction products.The development of high-performance catalysts is the key to the both electrocatalytic reactions.In this review,we present a systematic summary of the reaction systems for electrocatalytic CO_(2) reduction,along with the coupling mechanisms of C-C and C-N bonds over outstanding electrocatalytic materials recently developed.The key intermediate species and reaction pathways related to the coupling as well as the catalyst-structure relationship will be also discussed,aiming to provide insights and guidance for designing efficient CO_(2) reduction systems.展开更多
目前广泛应用的含Cr的薄膜有Cr N薄膜,以及以Cr N薄膜为基础,通过添加Si和C元素形成的Cr Si N薄膜、Cr CN薄膜和Cr Si CN薄膜。综述上述4种薄膜的结构及其力学和摩擦学特性的研究进展,阐述在不同摩擦环境下掺杂元素含量对薄膜摩擦因数...目前广泛应用的含Cr的薄膜有Cr N薄膜,以及以Cr N薄膜为基础,通过添加Si和C元素形成的Cr Si N薄膜、Cr CN薄膜和Cr Si CN薄膜。综述上述4种薄膜的结构及其力学和摩擦学特性的研究进展,阐述在不同摩擦环境下掺杂元素含量对薄膜摩擦因数和磨损率的影响,指出Si和C元素的掺杂均能改善Cr N薄膜的摩擦学性能,并从结构角度分析其原因。展开更多
采用热裂解聚合物前驱体法制备出了具有竹节结构的Si B C N纳米材料。扫描电子显微镜(SEM)和透射电子显微镜(TEM)结果表明样品具有特殊的竹节状(叠杯状)形貌,电子散射能谱(EDX)证实了样品组分为Si、B、C、N。通过微区喇曼光谱仪研究了...采用热裂解聚合物前驱体法制备出了具有竹节结构的Si B C N纳米材料。扫描电子显微镜(SEM)和透射电子显微镜(TEM)结果表明样品具有特殊的竹节状(叠杯状)形貌,电子散射能谱(EDX)证实了样品组分为Si、B、C、N。通过微区喇曼光谱仪研究了样品在488nm激光激发下从84～290K的变温发射特性,在490～800nm观察到位于580,620nm附近两个较强发射峰和740nm附近一个弱的发射峰。变温实验说明相应发射峰与材料禁带中形成的杂质能级有关。展开更多
基金supported by the Research Grants Council(26206115,16304821 and 16309418)the Southern Marine Science and Engineering Guangdong Laboratory(Guangzhou)(SMSEGL20SC01)+2 种基金the Innovation and Technology Commission(grant no.ITC-CNERC14EG03)of the Hong Kong Special Administrative Regionthe Hong Kong Postdoctoral Fellowship Scheme(HKUST PDFS2021-4S12 and HKUST PDFS2021-6S08)the support from the Shenzhen fundamental research funding(JCYJ20210324115809026,20200925154115001,JCYJ20200109141216566)。
文摘Urea generation through electrochemical CO_(2) and NO_(3)~-co-reduction reaction(CO_(2)NO_(3)RR)is still limited by either the low selectivity or yield rate of urea.Herein,we report copper carbonate hydroxide(Cu_2(OH)_2CO_(3))as an efficient CO_(2)NO_(3)RR electrocatalyst with an impressive urea Faradaic efficiency of45.2%±2.1%and a high yield rate of 1564.5±145.2μg h~(-1)mg_(cat)~(-1).More importantly,H_(2) evolution is fully inhibited on this electrocatalyst over a wide potential range between-0.3 and-0.8 V versus reversible hydrogen electrode.Our thermodynamic simulation reveals that the first C-N coupling follows a unique pathway on Cu_2(OH)_2CO_(3) by combining the two intermediates,~*COOH and~*NHO.This work demonstrates that high selectivity and yield rate of urea can be simultaneously achieved on simple Cu-based electrocatalysts in CO_(2)NO_(3)RR,and provide guidance for rational design of more advanced catalysts.
基金support from the Tangshan Talent Funding Project(Grant No.A202202007)National Natural Science Foundation of China(Grant Nos.22102136 and 21703065)+2 种基金Natural Science Foundation of Hebei Province(Grant Nos.B2018209267 and E2022209039)Natural Science Foundation of Hubei Province(Grant No.2022CFB1001)Department of Education of Hubei Province(Grant No.Q20221701).
文摘Electrochemical C-C and C-N coupling reactions with the conversion of abundant and inexpensive small molecules,such as CO_(2) and nitrogencontaining species,are considered a promising route for increasing the value of CO_(2) reduction products.The development of high-performance catalysts is the key to the both electrocatalytic reactions.In this review,we present a systematic summary of the reaction systems for electrocatalytic CO_(2) reduction,along with the coupling mechanisms of C-C and C-N bonds over outstanding electrocatalytic materials recently developed.The key intermediate species and reaction pathways related to the coupling as well as the catalyst-structure relationship will be also discussed,aiming to provide insights and guidance for designing efficient CO_(2) reduction systems.
文摘目前广泛应用的含Cr的薄膜有Cr N薄膜,以及以Cr N薄膜为基础,通过添加Si和C元素形成的Cr Si N薄膜、Cr CN薄膜和Cr Si CN薄膜。综述上述4种薄膜的结构及其力学和摩擦学特性的研究进展,阐述在不同摩擦环境下掺杂元素含量对薄膜摩擦因数和磨损率的影响,指出Si和C元素的掺杂均能改善Cr N薄膜的摩擦学性能,并从结构角度分析其原因。
文摘采用热裂解聚合物前驱体法制备出了具有竹节结构的Si B C N纳米材料。扫描电子显微镜(SEM)和透射电子显微镜(TEM)结果表明样品具有特殊的竹节状(叠杯状)形貌,电子散射能谱(EDX)证实了样品组分为Si、B、C、N。通过微区喇曼光谱仪研究了样品在488nm激光激发下从84～290K的变温发射特性,在490～800nm观察到位于580,620nm附近两个较强发射峰和740nm附近一个弱的发射峰。变温实验说明相应发射峰与材料禁带中形成的杂质能级有关。
