Tremendous efforts have been devoted to explore energy-efficient strategies of ammonia synthesis to replace Haber-Bosch process which accounts for 1.4% of the annual energy consumption. In this study, atomically dispe...Tremendous efforts have been devoted to explore energy-efficient strategies of ammonia synthesis to replace Haber-Bosch process which accounts for 1.4% of the annual energy consumption. In this study, atomically dispersed Au_1 catalyst is synthesized and applied in electrochemical synthesis of ammonia under ambient conditions. A high NH＋4 Faradaic efficiency of 11.1 % achieved by our Au_1 catalyst surpasses most of reported catalysts under comparable conditions. Benefiting from efficient atom utilization, an NH＋4 yield rate of 1,305 μg h-1 mg-1Au has been reached, which is roughly 22.5 times as high as that by sup- ported Au nanoparticles. We also demonstrate that by employing our Au_1 catalyst, NH＋4 can be electro- chemically produced directly from N_2 and H_2 with an energy utilization rate of 4.02 mmol kJ-1. Our study provides a possibility of replacing the Haber-Bosch process with environmentally benign and energy-efficient electrochemical strategies.展开更多
Printing techniques hold great potential in the manufacture of electronics such as sensors,micro-supercapacitors,and flexible electronics.However,developing large-scale functional conductive inks with appropriate rheo...Printing techniques hold great potential in the manufacture of electronics such as sensors,micro-supercapacitors,and flexible electronics.However,developing large-scale functional conductive inks with appropriate rheological properties and active components still remains a challenge.Herein,through optimizing the formulations of ink,iron single sites supported N-doped carbon black(Fe_(1)-NC)inks can serve as both conductive electrodes and high-reactive catalysts to realize convenient glucose detection,which pronouncedly reduces the dosage of enzyme and simplifies the sensors preparation.In detail,utilizing in-situ pyrolysis method,Fe_(1)-NC single-atom catalysts(SACs)are prepared in bulk(dekagram-level).The batched Fe_(1)-NC SACs materials can be uniformly mixed with modulated ink to realize the screen printing with high resolution and uniformity.Also,the whole scalable preparation and ink-functional process can be extended to various metals(including Co,Ni,Cu,and Mn).The introduction of highly active Fe_(1)-NC sites reduces the amount of enzyme used in glucose detection by at least 50%,contributing to the cost reduction of sensors.The strategy in harnessing the SACs onto the carbon inks thus provides a broad prospect for the low-cost and large-scale printing of sensitive sensing devices.展开更多
Engineering the local three-dimensional structure of metal sites has an important effect of maximizing the activity and selectivity of single-atom site catalysts.Here,we engineered a strain-assisted single Pt sites st...Engineering the local three-dimensional structure of metal sites has an important effect of maximizing the activity and selectivity of single-atom site catalysts.Here,we engineered a strain-assisted single Pt sites structure on a highly curved MoS_(2)surface to enhance its H_(2)S sensor property.By introducing N-methyl-2-pyrrolidone(NMP)as guiding molecules,a multilayer MoS_(2)structure with bending base planes was achieved.This bending behavior could inject not only uniform in-plane strain into the original inert MoS_(2)basal plane but also introduce sufficient accessible sites to anchor Pt monomers.Further experimental and theoretical results showed that the highcurvature MoS_(2)surface endowed 0.8%stretch strain onto the low-coordinated single Pt sites with a unique“tip”effect,which led to more accumulation of electrons around the Pt species,thereby accelerating the electric transfer process between H_(2)S and supports.The final catalyst delivered pronouncedly enhanced H_(2)S sensing response and response speed at room temperature.Our proposed strain-assisted strategy might create a new path to design highly active single-atom site catalysts for gas sensors.展开更多
基金supported by the National Key R&D Program of China (2017YFA0208300)the National Natural Science Foundation of China (21522107, 21671180, 21521091, 21390393, U1463202, and 21522305)
文摘Tremendous efforts have been devoted to explore energy-efficient strategies of ammonia synthesis to replace Haber-Bosch process which accounts for 1.4% of the annual energy consumption. In this study, atomically dispersed Au_1 catalyst is synthesized and applied in electrochemical synthesis of ammonia under ambient conditions. A high NH＋4 Faradaic efficiency of 11.1 % achieved by our Au_1 catalyst surpasses most of reported catalysts under comparable conditions. Benefiting from efficient atom utilization, an NH＋4 yield rate of 1,305 μg h-1 mg-1Au has been reached, which is roughly 22.5 times as high as that by sup- ported Au nanoparticles. We also demonstrate that by employing our Au_1 catalyst, NH＋4 can be electro- chemically produced directly from N_2 and H_2 with an energy utilization rate of 4.02 mmol kJ-1. Our study provides a possibility of replacing the Haber-Bosch process with environmentally benign and energy-efficient electrochemical strategies.
基金supported by the Ministry of Science and Technology of China(No.2021YFA1500404)the National Natural Science Foundation of China(Nos.92261105 and 22221003)+1 种基金USTC Research Funds of the Double First-Class Initiative(No.YD9990002022)the Shanghai Sailing Program(No.22YF1413400).
文摘Printing techniques hold great potential in the manufacture of electronics such as sensors,micro-supercapacitors,and flexible electronics.However,developing large-scale functional conductive inks with appropriate rheological properties and active components still remains a challenge.Herein,through optimizing the formulations of ink,iron single sites supported N-doped carbon black(Fe_(1)-NC)inks can serve as both conductive electrodes and high-reactive catalysts to realize convenient glucose detection,which pronouncedly reduces the dosage of enzyme and simplifies the sensors preparation.In detail,utilizing in-situ pyrolysis method,Fe_(1)-NC single-atom catalysts(SACs)are prepared in bulk(dekagram-level).The batched Fe_(1)-NC SACs materials can be uniformly mixed with modulated ink to realize the screen printing with high resolution and uniformity.Also,the whole scalable preparation and ink-functional process can be extended to various metals(including Co,Ni,Cu,and Mn).The introduction of highly active Fe_(1)-NC sites reduces the amount of enzyme used in glucose detection by at least 50%,contributing to the cost reduction of sensors.The strategy in harnessing the SACs onto the carbon inks thus provides a broad prospect for the low-cost and large-scale printing of sensitive sensing devices.
基金This work was supported by the China Ministry of Science and Technology(grant no.2020YFA0710200)National Key R&D Program of China 2017YFA(grant nos.0208300 and 0700104)+2 种基金the National Natural Science Foundation of China(grant no.21671180)the Dalian National Laboratory for Clean Energy(DNL)Cooperation Fund,CAS(grant no.DNL201918)the Fundamental Research Funds for the Central Universities(grant nos.WK2060120004,WK2060000021,WK2060000025,and KY2060000180).
文摘Engineering the local three-dimensional structure of metal sites has an important effect of maximizing the activity and selectivity of single-atom site catalysts.Here,we engineered a strain-assisted single Pt sites structure on a highly curved MoS_(2)surface to enhance its H_(2)S sensor property.By introducing N-methyl-2-pyrrolidone(NMP)as guiding molecules,a multilayer MoS_(2)structure with bending base planes was achieved.This bending behavior could inject not only uniform in-plane strain into the original inert MoS_(2)basal plane but also introduce sufficient accessible sites to anchor Pt monomers.Further experimental and theoretical results showed that the highcurvature MoS_(2)surface endowed 0.8%stretch strain onto the low-coordinated single Pt sites with a unique“tip”effect,which led to more accumulation of electrons around the Pt species,thereby accelerating the electric transfer process between H_(2)S and supports.The final catalyst delivered pronouncedly enhanced H_(2)S sensing response and response speed at room temperature.Our proposed strain-assisted strategy might create a new path to design highly active single-atom site catalysts for gas sensors.
