The development of a highly efficient catalyst for CO_(2) activation and selective conversion to methanol is critical to address the issues associated with the high thermal stability of CO_(2) and controllable synthes...The development of a highly efficient catalyst for CO_(2) activation and selective conversion to methanol is critical to address the issues associated with the high thermal stability of CO_(2) and controllable synthesis of methanol.Cu-based catalysts have been widely studied because of the low cost and excellent performance in mild conditions.However,the improvement of catalytic activity and selectivity remains challenging.Herein,we prepared hollow Cu@ZrO_(2) catalysts through pyrolysis of Cu-loaded Zr-MOF for CO_(2) hydrogenation to methanol.Low-temperature pyrolysis generated highly dispersed Cu nanoparticles with balanced Cu^(0)/Cu^(+)sites,larger amounts of surface basic sites and abundant Cu-ZrO_(2) interface in the hollow structure,contributing to enhanced catalytic capacity for adsorption/activation of CO_(2) and selective hydrogenation to methanol.In situ Fourier Transform Infrared Spectroscopy revealed the methanol formation followed the formate-intermediated pathway.This work would provide a guideline for the design of high-performance catalysts and the understanding of the mechanism and active sites for CO_(2) hydrogenation to methanol.展开更多
Powered by electricity from renewable energies,electrochemical reduction of CO_(2)could not only efficiently alleviate the excess emission of CO_(2),but also produce many kinds of valuable chemical feedstocks.Among va...Powered by electricity from renewable energies,electrochemical reduction of CO_(2)could not only efficiently alleviate the excess emission of CO_(2),but also produce many kinds of valuable chemical feedstocks.Among various catalysts,single atom catalysts(SACs)have attracted much attention due to their high atom utilization efficiency and expressive catalytic performances.Additionally,SACs serve as an ideal platform for the investigation of complex reaction pathways and mechanisms thanks to their explicit active sites.In this review,the possible re-action pathways for the generation of various products(mainly C1 products for SACs)were firstly summarized.Then,recent progress of SACs for electrochemical reduction of CO_(2)was discussed in aspect of different central metal sites.As the most popular and efficient coordination modulation strategy,introducing heteroatom was then reviewed.Moreover,as an extension of SACs,the development of dual atom catalysts was also briefly discussed.At last,some issues and challenges regarding the SACs for CO_(2)reduction reaction(CO_(2)RR)were listed,followed by corresponding suggestions.展开更多
SnO2 grafted MCM-41 sensor was prepared by MOCVD in the pore of MCM-41. The sensor has high sensitivity for carbon monoxide at low temperature compared with commercially available low-surface-area tin dioxide.
Bifunctional oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)electrocatalysts with the advantages of excellent activity and stability are the vital components of air cathodes for rechargeable Zn–air b...Bifunctional oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)electrocatalysts with the advantages of excellent activity and stability are the vital components of air cathodes for rechargeable Zn–air batteries(ZABs).Herein,the carbon aerogel with honeycomb-like structure,N and S double doping and loaded with FeCo alloy nanoparticles(NSCA/FeCo)was prepared successfully as cathodes for rechargeable liquid flow and two-dimensional flexible ZABs by clever directional casting.The interaction between the bimetallic alloy and the double-doped carbon with specifical structure,large surface,great conductivity endows NSCA/FeCo with effective ORR/OER active sites and small charge/mass transport barrier,thus achieving outstanding bifunctional catalytic performance.The NSCA/FeCo displays a half-wave potential of+0.85 V(vs.reversible hydrogen electrode(RHE))for ORR and an overpotential of 335 mV at a current density of 10 mA·cm^(−2)for OER,which is even comparable to the performance of noble-metal catalysts in relevant fields(Pt/C for ORR and RuO_(2)for OER).Consequently,the rechargeable liquid flow ZABs assembled with NSCA/FeCo showed excellent performance(maximum power density:132.0 mW·cm^(−2),specific capacity:804.5 Wh·kg^(−1)at 10 mA·cm^(−2),charge and discharge cycle stability of more than 250 cycles).Furthermore,the flexible NSCA/FeCo-based ZABs have a maximum power density of 43.0 mW·cm^(−2),outstanding charging–discharge stability of more than 450 cycles,exhibit good flexibility under different bending conditions.Therefore,this work has provided an efficient bifunctional electrocatalyst for OER/ORR and a promising strategy of air cathodes for rechargeable and wearable ZABs.展开更多
In the past decades,machine learning(ML)has impacted the field of electrocatalysis.Modern researchers have begun to take advantage of ML‐based data‐driven techniques to overcome the computational and experimental li...In the past decades,machine learning(ML)has impacted the field of electrocatalysis.Modern researchers have begun to take advantage of ML‐based data‐driven techniques to overcome the computational and experimental limitations to accelerate rational catalyst design.Hence,significant efforts have been made to perform ML to accelerate calculation and aid electrocatalyst design for CO_(2) reduction.This review discusses recent applications of ML to discover,design,and optimize novel electrocatalysts.First,insights into ML aided in accelerating calculation are presented.Then,ML aided in the rational design of the electrocatalyst is introduced,including establishing a data set/data source selection and validation of descriptor selection of ML algorithms validation and predictions of the model.Finally,the opportunities and future challenges are summarized for the future design of electrocatalyst for CO_(2) reduction with the assistance of ML.展开更多
基金the financial support by the National Natural Science Foundation of China(22178265,U21B2096,21938008)the Tianjin Key Science and Technology Project(19ZXNCGX00030)。
文摘The development of a highly efficient catalyst for CO_(2) activation and selective conversion to methanol is critical to address the issues associated with the high thermal stability of CO_(2) and controllable synthesis of methanol.Cu-based catalysts have been widely studied because of the low cost and excellent performance in mild conditions.However,the improvement of catalytic activity and selectivity remains challenging.Herein,we prepared hollow Cu@ZrO_(2) catalysts through pyrolysis of Cu-loaded Zr-MOF for CO_(2) hydrogenation to methanol.Low-temperature pyrolysis generated highly dispersed Cu nanoparticles with balanced Cu^(0)/Cu^(+)sites,larger amounts of surface basic sites and abundant Cu-ZrO_(2) interface in the hollow structure,contributing to enhanced catalytic capacity for adsorption/activation of CO_(2) and selective hydrogenation to methanol.In situ Fourier Transform Infrared Spectroscopy revealed the methanol formation followed the formate-intermediated pathway.This work would provide a guideline for the design of high-performance catalysts and the understanding of the mechanism and active sites for CO_(2) hydrogenation to methanol.
文摘Powered by electricity from renewable energies,electrochemical reduction of CO_(2)could not only efficiently alleviate the excess emission of CO_(2),but also produce many kinds of valuable chemical feedstocks.Among various catalysts,single atom catalysts(SACs)have attracted much attention due to their high atom utilization efficiency and expressive catalytic performances.Additionally,SACs serve as an ideal platform for the investigation of complex reaction pathways and mechanisms thanks to their explicit active sites.In this review,the possible re-action pathways for the generation of various products(mainly C1 products for SACs)were firstly summarized.Then,recent progress of SACs for electrochemical reduction of CO_(2)was discussed in aspect of different central metal sites.As the most popular and efficient coordination modulation strategy,introducing heteroatom was then reviewed.Moreover,as an extension of SACs,the development of dual atom catalysts was also briefly discussed.At last,some issues and challenges regarding the SACs for CO_(2)reduction reaction(CO_(2)RR)were listed,followed by corresponding suggestions.
文摘SnO2 grafted MCM-41 sensor was prepared by MOCVD in the pore of MCM-41. The sensor has high sensitivity for carbon monoxide at low temperature compared with commercially available low-surface-area tin dioxide.
基金the Fundamental Research Funds for the Central Universities(No.30920041108).
文摘Bifunctional oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)electrocatalysts with the advantages of excellent activity and stability are the vital components of air cathodes for rechargeable Zn–air batteries(ZABs).Herein,the carbon aerogel with honeycomb-like structure,N and S double doping and loaded with FeCo alloy nanoparticles(NSCA/FeCo)was prepared successfully as cathodes for rechargeable liquid flow and two-dimensional flexible ZABs by clever directional casting.The interaction between the bimetallic alloy and the double-doped carbon with specifical structure,large surface,great conductivity endows NSCA/FeCo with effective ORR/OER active sites and small charge/mass transport barrier,thus achieving outstanding bifunctional catalytic performance.The NSCA/FeCo displays a half-wave potential of+0.85 V(vs.reversible hydrogen electrode(RHE))for ORR and an overpotential of 335 mV at a current density of 10 mA·cm^(−2)for OER,which is even comparable to the performance of noble-metal catalysts in relevant fields(Pt/C for ORR and RuO_(2)for OER).Consequently,the rechargeable liquid flow ZABs assembled with NSCA/FeCo showed excellent performance(maximum power density:132.0 mW·cm^(−2),specific capacity:804.5 Wh·kg^(−1)at 10 mA·cm^(−2),charge and discharge cycle stability of more than 250 cycles).Furthermore,the flexible NSCA/FeCo-based ZABs have a maximum power density of 43.0 mW·cm^(−2),outstanding charging–discharge stability of more than 450 cycles,exhibit good flexibility under different bending conditions.Therefore,this work has provided an efficient bifunctional electrocatalyst for OER/ORR and a promising strategy of air cathodes for rechargeable and wearable ZABs.
基金ANU Futures Scheme,Grant/Award Number:Q4601024National Natural Science Foundation of China,Grant/Award Number:22078054+1 种基金Australian Research Council,Grant/Award Number:DP190100295China Scholarship Council(CSC)Program。
文摘In the past decades,machine learning(ML)has impacted the field of electrocatalysis.Modern researchers have begun to take advantage of ML‐based data‐driven techniques to overcome the computational and experimental limitations to accelerate rational catalyst design.Hence,significant efforts have been made to perform ML to accelerate calculation and aid electrocatalyst design for CO_(2) reduction.This review discusses recent applications of ML to discover,design,and optimize novel electrocatalysts.First,insights into ML aided in accelerating calculation are presented.Then,ML aided in the rational design of the electrocatalyst is introduced,including establishing a data set/data source selection and validation of descriptor selection of ML algorithms validation and predictions of the model.Finally,the opportunities and future challenges are summarized for the future design of electrocatalyst for CO_(2) reduction with the assistance of ML.