Hierarchical lignin-derived ordered mesoporous carbon(HOMC)was significant for advanced supercapacitors.However,achieving controllable fabrication and optimizing electrochemical behavior were challenging.In this work,...Hierarchical lignin-derived ordered mesoporous carbon(HOMC)was significant for advanced supercapacitors.However,achieving controllable fabrication and optimizing electrochemical behavior were challenging.In this work,an eco-friendly HOMC was synthesized using lignin as carbon precursors and Zn^(2+)as cross-linking and pore-forming agents,followed by KHCO_(3)activation,eliminating the need for toxic phenolic resins and acid treatments for metal removal.Machine learning technology,specifically an Artificial Neural Network(ANN model,was utilized to assist the experimental design and prediction.The ANN model suggested an ideal hierarchical structure and optimized oxygen level,achieved through the adjustment of Zn^(2+)additive concentration,carbonization temperature,and subsequent KHCO_(3)activation to maximize capacitance.The HOMC electrode,with a micropore-to-mesopore ratio(S_(micro)/S_(meso))of 1.01 and an oxygen content of 8.81 at%,acquired a specific capacitance of 362 F·g^(-1)at 0.5 A·g^(-1)in 6 mol·L^(-1)KOH electrolyte.The assembled HOMC//HOMC supercapacitor could afford a high energy density of 33.38 Wh·kg^(-1)with a corresponding specific power density of 300 W·kg^(-1)in TEATFB PC electrolyte.Meanwhile,the long-term cycle stability of 94.33%was achieved after 20,000 cycles.This work provides an ANN assisted strategy for the synthesis of HOMC,highlighting its potential to valorize biomass and agricultural waste in sustainable energy storag solutions.展开更多
Developing host materials with high specific surface area, good electron conductivity, and fast ion transportation channel is critical for high performance lithium-selenium(Li-Se) batteries. Herein, a series of three ...Developing host materials with high specific surface area, good electron conductivity, and fast ion transportation channel is critical for high performance lithium-selenium(Li-Se) batteries. Herein, a series of three dimensional ordered hierarchically porous carbon(3D OHPC) materials with micro/meso/macropores are designed and synthesized for Li-Se battery. The porous structure is tuned by following the concept of the generalized Murray’s law to facilitate the mass diffusion and reduce ion transport resistance.The optimized 3D Se/OHPC cathode exhibits a very high 2 nd discharge capacity of 651 m Ah/g and retains 361 m Ah/g after 200 cycles at 0.2 C. Even at a high current rate of 5 C, the battery still shows a discharge capacity as high as 155 m Ah/g. The improved electrochemical performance is attributed to the synergy effect of the interconnected and well-designed micro, meso and macroporosity while shortened ions diffusion pathways of such Murray materials accelerate its ionic and electronic conductivities leading to the enhanced electrochemical reaction. The diffusivity coefficient in Se/OHPC can reach a very high value of 1.3 × 10^(-11)cm^(2)/s, much higher than those in single pore size carbon hosts. Their effective volume expansion accommodation capability and reduced dissolution of polyselenides ensure the high stability of the battery. This work, for the first time, established the clear relationship between textural properties of cathode materials and their performance and demonstrates that the concept of the generalized Murray’s law can be used as efficient guidance for the rational design and synthesis of advanced hierarchically porous materials and the great potential of 3D OHPC materials as a practical high performance cathode material for Li-Se batteries.展开更多
AIM:To evaluate long-term visual field(VF)prediction using K-means clustering in patients with primary open angle glaucoma(POAG).METHODS:Patients who underwent 24-2 VF tests≥10 were included in this study.Using 52 to...AIM:To evaluate long-term visual field(VF)prediction using K-means clustering in patients with primary open angle glaucoma(POAG).METHODS:Patients who underwent 24-2 VF tests≥10 were included in this study.Using 52 total deviation values(TDVs)from the first 10 VF tests of the training dataset,VF points were clustered into several regions using the hierarchical ordered partitioning and collapsing hybrid(HOPACH)and K-means clustering.Based on the clustering results,a linear regression analysis was applied to each clustered region of the testing dataset to predict the TDVs of the 10th VF test.Three to nine VF tests were used to predict the 10th VF test,and the prediction errors(root mean square error,RMSE)of each clustering method and pointwise linear regression(PLR)were compared.RESULTS:The training group consisted of 228 patients(mean age,54.20±14.38y;123 males and 105 females),and the testing group included 81 patients(mean age,54.88±15.22y;43 males and 38 females).All subjects were diagnosed with POAG.Fifty-two VF points were clustered into 11 and nine regions using HOPACH and K-means clustering,respectively.K-means clustering had a lower prediction error than PLR when n=1:3 and 1:4(both P≤0.003).The prediction errors of K-means clustering were lower than those of HOPACH in all sections(n=1:4 to 1:9;all P≤0.011),except for n=1:3(P=0.680).PLR outperformed K-means clustering only when n=1:8 and 1:9(both P≤0.020).CONCLUSION:K-means clustering can predict longterm VF test results more accurately in patients with POAG with limited VF data.展开更多
Highway work zones are locations where severe traffic crashes tend to occur.Most of the extant research on work zone crash severity neglects the discrepancy in the injuries sustained by different drivers involved in t...Highway work zones are locations where severe traffic crashes tend to occur.Most of the extant research on work zone crash severity neglects the discrepancy in the injuries sustained by different drivers involved in the same crash.Admittedly,it is essential to analyse crash-level factors to their highest injury severity;but it is equally important to understand driver-level contributing factors to their injury severity to establish effective safety countermeasures to minimize drivers’injury severity.Thus,this research aims to identify the factors with significant impacts on the driver injury severity of work zone crashes and estimate their effects on each severity level.Data on 3880 drivers involved in 2134 work zone crashes are obtained from the Crash Report Sampling System(CRSS)database of the United States and employed for the empirical investigation.A Bayesian hierarchical generalized ordered probit model is advocated for analysing the driver injury severity.Model performance indices suggest that the advocated hierarchical model is superior to the generalized ordered probit model,and considerable within-crash correlation is found across the observed driver injury severity.The estimated parameters show that driver age and sex,alcohol use,vehicle age and type,speeding and speed limit,weather conditions,lighting conditions and crash type have significant effects on the driver injury severity in work zone crashes.Marginal effects of the significant factors on each divided injury severity level are also estimated.Countermeasures are proposed from the results to reduce severe injuries sustained by drivers involved in work zone crashes.展开更多
Utilization of carbon-based materials is crucial for mitigating CO_(2) emissions.However,practical materials for CO_(2) capture remain challenging due to limitations in adsorption capacity and rate.Inspired by the uni...Utilization of carbon-based materials is crucial for mitigating CO_(2) emissions.However,practical materials for CO_(2) capture remain challenging due to limitations in adsorption capacity and rate.Inspired by the unique structural features of biomass materials,high-performance hierarchical porous carbon was prepared using vascular plants.The ordered arrangement structure effectively improved the adsorption capacity and rate of the material by optimizing the pore structure.Potassium hydroxide(KOH)was used as an activator to synthesize microporous carbon with an ordered hierarchical structure.The properties of hierarchical porous carbon were characterized.The experimental results indicate that porous carbon prepared from loofah complex has excellent CO_(2) adsorption capacity.The highest adsorption capacity is 4.09 mmol/g when the activation temperature is 700℃.The selectivity(15/85)for the binary gas mixture CO_(2)/N_(2) was 20,and the recoverability was good after 10 cycles.The hierarchical porous carbon derived from loofah showed excellent adsorption performance and has potential in various applications.展开更多
The development of novel nanozymes for environmental contamination remediation is a worthwhile research direction.However,most of the reported nanozymes cannot degrade efficiently due to the limitation of the internal...The development of novel nanozymes for environmental contamination remediation is a worthwhile research direction.However,most of the reported nanozymes cannot degrade efficiently due to the limitation of the internal active sites not being able to come into direct contact with contaminants.Therefore,we reported Fe-N-C single-atom nanozymes(SAzymes)with atomically dispersed FeN4 active sites anchored on a three-dimensional hierarchically ordered microporous-mesoporous-macroporous nitrogen doped carbon matrix(3DOM Fe-N-C)for the degradation of a targeted environmental pollutant(rhodamine B(RhB)).The three-dimensional(3D)hierarchically ordered porous structure may accelerate mass transfer and improve the accessibility of active sites.This structure and high metal atom utilization endow Fe-N-C SAzyme with enhanced tri-enzyme-mimic activities,comprising oxidase-mimic,peroxidase-mimic,and catalase-mimic activities.Based on its excellent peroxidase-mimic activity,3DOM Fe-N-C can degrade RhB by hydroxyl radicals(·OH)generated in the presence of hydrogen peroxide.This study provides a new idea for designing porous Fe-N-C SAzymes for environmental contamination remediation.展开更多
Maximizing the fixing ability of polyselenides to reduce the shuttle effect in Li-Se batteries remains highly challenging.Single crystal metal-organic framework(MOF)-derived N-doped ordered hierarchically porous carbo...Maximizing the fixing ability of polyselenides to reduce the shuttle effect in Li-Se batteries remains highly challenging.Single crystal metal-organic framework(MOF)-derived N-doped ordered hierarchically porous carbon(SNOHPC)synthesized by a confined crystal growth and template-assisted method demonstrates excellent electrochemical performance as a host material for Li-Se battery.The large number of micropores inherited from the MOF structure provides large space and surface for Se loading and reaction sites,ensuring the high energy density of the battery.The insitu X-ray diffraction(XRD)technique is used to understand the reaction mechanism.The synergy of the interconnected three-scale-level micro-meso-macroporous structure and Ndoped polar sites can buffer the volume expansion,shorten the ion transportation with a very high diffusion coefficient of4.44×10cm^(2)sand accelerate the lithiation/delithiation reaction.Selenium is sufficiently reactive and the polyselenide intermediates are tightly fixed inside the carbon host material,thereby achieving excellent specific capacity,stability,and rate capability.Such a cathode exhibits a very high 2discharge/charge capacity of 658 and 683 mA h g,respectively,and retains a very high capacity of 367 mA h gafter 200 cycles at the current of 0.2 C.Even at the high current of 5 C,a very high discharge capacity of 230 mA h gis obtained.This work provides a new kind of high-performance porous materials with rational pore arrangement applicable for highly efficient energy storage.展开更多
Microporous supports typically fail to fully expose active sites for electrolytes and CO_(2) molecules,and this usually results in low current density for the electrocatalytic CO_(2) reduction reaction(CO_(2)RR).To ov...Microporous supports typically fail to fully expose active sites for electrolytes and CO_(2) molecules,and this usually results in low current density for the electrocatalytic CO_(2) reduction reaction(CO_(2)RR).To overcome the biggest obstacle and facilitate commercial applications,defective single-atomic Ni-N_(3) sites anchored to ordered micro-macroporous N-doped carbon(Ni-N/OMC)have been prepared by the pyrolysis of the Ni-ZIF-8@PS(ZIF=zeolitic imidazolate framework)and are intended to provide enhanced CO_(2)RR with a current density at an industrial level.This Ni-ZIF-8@PS is constructed of nickel-based ZIF-8 embedded in the three-dimensional(3D)highly ordered polystyrene spheres(PS).The 3D ordered micro-macroporous architecture of Ni-N/OMC could facilitate the mass transfer of substrates to the accessible defective single-atomic Ni-N_(3) sites through micropores(0.6 nm)and macropores(~200 nm)interconnected by 50 nm channels.In a flow cell,Ni-N/OMC exhibits almost 100.0%CO Faraday efficiency(FECO)between−0.2 and−1.1 V vs.RHE and an industrial level CO partial current density of 208 mA cm^(−2).It has a turnover frequency of 1.5×10^(5) h^(−1) at−1.1 V vs.RHE in 1 M KOH electrolyte,which exceeds that of most reported nickel-based electrocatalysts.This excellent CO_(2)RR performance for Ni-N/OMC makes it a state-of-the-art electrocatalyst for CO_(2)RR.Theoretical calculations show that the defective Ni-N_(3) site can lower the energy of*COOH formation compared with that of the Ni-N4 site,thereby accelerating CO_(2)RR.Ni-N/OMC can also be utilized as a cathodic catalyst in Zn-CO_(2) battery,exhibiting high CO selectivity in the discharge process and excellent stability.This work paves a pathway to rational design of highly efficient electrocatalysts with 3D hierarchically ordered micro-macroporous architecture for CO_(2)RR towards industrial production and commercial applications.展开更多
基金supported by National Natural Science Foundation of China(52376104,52201158)Joint Funds of the National Natural Science Foundation of China(U20A20302)+3 种基金Innovative group projects in Hebei Province(E2021202006)the project of Science and Technology in the Universities of Hebei Province(JZX2023006)Natural Science Foundation of Hebei Province(C202202003)Hebei University of Technology Cross-disciplinary(XKJC-2024001)。
文摘Hierarchical lignin-derived ordered mesoporous carbon(HOMC)was significant for advanced supercapacitors.However,achieving controllable fabrication and optimizing electrochemical behavior were challenging.In this work,an eco-friendly HOMC was synthesized using lignin as carbon precursors and Zn^(2+)as cross-linking and pore-forming agents,followed by KHCO_(3)activation,eliminating the need for toxic phenolic resins and acid treatments for metal removal.Machine learning technology,specifically an Artificial Neural Network(ANN model,was utilized to assist the experimental design and prediction.The ANN model suggested an ideal hierarchical structure and optimized oxygen level,achieved through the adjustment of Zn^(2+)additive concentration,carbonization temperature,and subsequent KHCO_(3)activation to maximize capacitance.The HOMC electrode,with a micropore-to-mesopore ratio(S_(micro)/S_(meso))of 1.01 and an oxygen content of 8.81 at%,acquired a specific capacitance of 362 F·g^(-1)at 0.5 A·g^(-1)in 6 mol·L^(-1)KOH electrolyte.The assembled HOMC//HOMC supercapacitor could afford a high energy density of 33.38 Wh·kg^(-1)with a corresponding specific power density of 300 W·kg^(-1)in TEATFB PC electrolyte.Meanwhile,the long-term cycle stability of 94.33%was achieved after 20,000 cycles.This work provides an ANN assisted strategy for the synthesis of HOMC,highlighting its potential to valorize biomass and agricultural waste in sustainable energy storag solutions.
基金financial support from the China Scholarship Council (CSC) and a scholarship from the Laboratory of Inorganic Materials Chemistry,Universitéde Namur,Belgiumfinancially supported by the National Postdoctoral Program (Grant No. 2020M672782)+2 种基金the National Natural Science Foundation of China (Grant No. U1663225)the the Program of Introducing Talents of Discipline to Universities-National 111 Project from the Ministry of Science and Technology and the Ministry of Education of China (Grant No. B20002)the National Key R&D Program of China (Grant No. 2016YFA0202602)。
文摘Developing host materials with high specific surface area, good electron conductivity, and fast ion transportation channel is critical for high performance lithium-selenium(Li-Se) batteries. Herein, a series of three dimensional ordered hierarchically porous carbon(3D OHPC) materials with micro/meso/macropores are designed and synthesized for Li-Se battery. The porous structure is tuned by following the concept of the generalized Murray’s law to facilitate the mass diffusion and reduce ion transport resistance.The optimized 3D Se/OHPC cathode exhibits a very high 2 nd discharge capacity of 651 m Ah/g and retains 361 m Ah/g after 200 cycles at 0.2 C. Even at a high current rate of 5 C, the battery still shows a discharge capacity as high as 155 m Ah/g. The improved electrochemical performance is attributed to the synergy effect of the interconnected and well-designed micro, meso and macroporosity while shortened ions diffusion pathways of such Murray materials accelerate its ionic and electronic conductivities leading to the enhanced electrochemical reaction. The diffusivity coefficient in Se/OHPC can reach a very high value of 1.3 × 10^(-11)cm^(2)/s, much higher than those in single pore size carbon hosts. Their effective volume expansion accommodation capability and reduced dissolution of polyselenides ensure the high stability of the battery. This work, for the first time, established the clear relationship between textural properties of cathode materials and their performance and demonstrates that the concept of the generalized Murray’s law can be used as efficient guidance for the rational design and synthesis of advanced hierarchically porous materials and the great potential of 3D OHPC materials as a practical high performance cathode material for Li-Se batteries.
基金Supported by the Korea Health Technology R&D Project through the Korea Health Industry Development Institute(KHIDI),the Ministry of Health&Welfare,Republic of Korea(No.RS-2020-KH088726)the Patient-Centered Clinical Research Coordinating Center(PACEN),the Ministry of Health and Welfare,Republic of Korea(No.HC19C0276)the National Research Foundation of Korea(NRF),the Korea Government(MSIT)(No.RS-2023-00247504).
文摘AIM:To evaluate long-term visual field(VF)prediction using K-means clustering in patients with primary open angle glaucoma(POAG).METHODS:Patients who underwent 24-2 VF tests≥10 were included in this study.Using 52 total deviation values(TDVs)from the first 10 VF tests of the training dataset,VF points were clustered into several regions using the hierarchical ordered partitioning and collapsing hybrid(HOPACH)and K-means clustering.Based on the clustering results,a linear regression analysis was applied to each clustered region of the testing dataset to predict the TDVs of the 10th VF test.Three to nine VF tests were used to predict the 10th VF test,and the prediction errors(root mean square error,RMSE)of each clustering method and pointwise linear regression(PLR)were compared.RESULTS:The training group consisted of 228 patients(mean age,54.20±14.38y;123 males and 105 females),and the testing group included 81 patients(mean age,54.88±15.22y;43 males and 38 females).All subjects were diagnosed with POAG.Fifty-two VF points were clustered into 11 and nine regions using HOPACH and K-means clustering,respectively.K-means clustering had a lower prediction error than PLR when n=1:3 and 1:4(both P≤0.003).The prediction errors of K-means clustering were lower than those of HOPACH in all sections(n=1:4 to 1:9;all P≤0.011),except for n=1:3(P=0.680).PLR outperformed K-means clustering only when n=1:8 and 1:9(both P≤0.020).CONCLUSION:K-means clustering can predict longterm VF test results more accurately in patients with POAG with limited VF data.
基金supported by the Open Fund of the Key Laboratory of Highway Engineering of Ministry of Education(Changsha University of Science&Technology)(Grant No.kfj230301).
文摘Highway work zones are locations where severe traffic crashes tend to occur.Most of the extant research on work zone crash severity neglects the discrepancy in the injuries sustained by different drivers involved in the same crash.Admittedly,it is essential to analyse crash-level factors to their highest injury severity;but it is equally important to understand driver-level contributing factors to their injury severity to establish effective safety countermeasures to minimize drivers’injury severity.Thus,this research aims to identify the factors with significant impacts on the driver injury severity of work zone crashes and estimate their effects on each severity level.Data on 3880 drivers involved in 2134 work zone crashes are obtained from the Crash Report Sampling System(CRSS)database of the United States and employed for the empirical investigation.A Bayesian hierarchical generalized ordered probit model is advocated for analysing the driver injury severity.Model performance indices suggest that the advocated hierarchical model is superior to the generalized ordered probit model,and considerable within-crash correlation is found across the observed driver injury severity.The estimated parameters show that driver age and sex,alcohol use,vehicle age and type,speeding and speed limit,weather conditions,lighting conditions and crash type have significant effects on the driver injury severity in work zone crashes.Marginal effects of the significant factors on each divided injury severity level are also estimated.Countermeasures are proposed from the results to reduce severe injuries sustained by drivers involved in work zone crashes.
文摘Utilization of carbon-based materials is crucial for mitigating CO_(2) emissions.However,practical materials for CO_(2) capture remain challenging due to limitations in adsorption capacity and rate.Inspired by the unique structural features of biomass materials,high-performance hierarchical porous carbon was prepared using vascular plants.The ordered arrangement structure effectively improved the adsorption capacity and rate of the material by optimizing the pore structure.Potassium hydroxide(KOH)was used as an activator to synthesize microporous carbon with an ordered hierarchical structure.The properties of hierarchical porous carbon were characterized.The experimental results indicate that porous carbon prepared from loofah complex has excellent CO_(2) adsorption capacity.The highest adsorption capacity is 4.09 mmol/g when the activation temperature is 700℃.The selectivity(15/85)for the binary gas mixture CO_(2)/N_(2) was 20,and the recoverability was good after 10 cycles.The hierarchical porous carbon derived from loofah showed excellent adsorption performance and has potential in various applications.
基金We are grateful for the support from the Ministry of Science and Technology of China(Nos.2016YFA0203203 and 2019YFA0709202)the National Natural Science Foundation of China(No.22074137).
文摘The development of novel nanozymes for environmental contamination remediation is a worthwhile research direction.However,most of the reported nanozymes cannot degrade efficiently due to the limitation of the internal active sites not being able to come into direct contact with contaminants.Therefore,we reported Fe-N-C single-atom nanozymes(SAzymes)with atomically dispersed FeN4 active sites anchored on a three-dimensional hierarchically ordered microporous-mesoporous-macroporous nitrogen doped carbon matrix(3DOM Fe-N-C)for the degradation of a targeted environmental pollutant(rhodamine B(RhB)).The three-dimensional(3D)hierarchically ordered porous structure may accelerate mass transfer and improve the accessibility of active sites.This structure and high metal atom utilization endow Fe-N-C SAzyme with enhanced tri-enzyme-mimic activities,comprising oxidase-mimic,peroxidase-mimic,and catalase-mimic activities.Based on its excellent peroxidase-mimic activity,3DOM Fe-N-C can degrade RhB by hydroxyl radicals(·OH)generated in the presence of hydrogen peroxide.This study provides a new idea for designing porous Fe-N-C SAzymes for environmental contamination remediation.
基金the financial support from the China Scholarship Council(201809370046)a scholarship from the Laboratory of Inorganic Materials Chemistry Universitéde Namur+4 种基金supported by the National Postdoctoral Program(2020M672782)the National Natural Science Foundation of China(U1663225)Changjiang Scholars and Innovative Research Team in University(IRT_15R52)the Program of Introducing Talents of Discipline to Universities-Plan 111(B20002)from the Ministry of Science and Technology and the Ministry of Education of Chinathe National Key R&D Program of China(2016YFA0202602)。
文摘Maximizing the fixing ability of polyselenides to reduce the shuttle effect in Li-Se batteries remains highly challenging.Single crystal metal-organic framework(MOF)-derived N-doped ordered hierarchically porous carbon(SNOHPC)synthesized by a confined crystal growth and template-assisted method demonstrates excellent electrochemical performance as a host material for Li-Se battery.The large number of micropores inherited from the MOF structure provides large space and surface for Se loading and reaction sites,ensuring the high energy density of the battery.The insitu X-ray diffraction(XRD)technique is used to understand the reaction mechanism.The synergy of the interconnected three-scale-level micro-meso-macroporous structure and Ndoped polar sites can buffer the volume expansion,shorten the ion transportation with a very high diffusion coefficient of4.44×10cm^(2)sand accelerate the lithiation/delithiation reaction.Selenium is sufficiently reactive and the polyselenide intermediates are tightly fixed inside the carbon host material,thereby achieving excellent specific capacity,stability,and rate capability.Such a cathode exhibits a very high 2discharge/charge capacity of 658 and 683 mA h g,respectively,and retains a very high capacity of 367 mA h gafter 200 cycles at the current of 0.2 C.Even at the high current of 5 C,a very high discharge capacity of 230 mA h gis obtained.This work provides a new kind of high-performance porous materials with rational pore arrangement applicable for highly efficient energy storage.
基金supported by the National Key Research and Development Program of China(2018YFA0208600,2018YFA0704502)the National Science Foundation of China(21871263,22071245,22033008)+1 种基金the Youth Innovation Promotion Association,CAS(Y201850)Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China(2021ZZ103)。
文摘Microporous supports typically fail to fully expose active sites for electrolytes and CO_(2) molecules,and this usually results in low current density for the electrocatalytic CO_(2) reduction reaction(CO_(2)RR).To overcome the biggest obstacle and facilitate commercial applications,defective single-atomic Ni-N_(3) sites anchored to ordered micro-macroporous N-doped carbon(Ni-N/OMC)have been prepared by the pyrolysis of the Ni-ZIF-8@PS(ZIF=zeolitic imidazolate framework)and are intended to provide enhanced CO_(2)RR with a current density at an industrial level.This Ni-ZIF-8@PS is constructed of nickel-based ZIF-8 embedded in the three-dimensional(3D)highly ordered polystyrene spheres(PS).The 3D ordered micro-macroporous architecture of Ni-N/OMC could facilitate the mass transfer of substrates to the accessible defective single-atomic Ni-N_(3) sites through micropores(0.6 nm)and macropores(~200 nm)interconnected by 50 nm channels.In a flow cell,Ni-N/OMC exhibits almost 100.0%CO Faraday efficiency(FECO)between−0.2 and−1.1 V vs.RHE and an industrial level CO partial current density of 208 mA cm^(−2).It has a turnover frequency of 1.5×10^(5) h^(−1) at−1.1 V vs.RHE in 1 M KOH electrolyte,which exceeds that of most reported nickel-based electrocatalysts.This excellent CO_(2)RR performance for Ni-N/OMC makes it a state-of-the-art electrocatalyst for CO_(2)RR.Theoretical calculations show that the defective Ni-N_(3) site can lower the energy of*COOH formation compared with that of the Ni-N4 site,thereby accelerating CO_(2)RR.Ni-N/OMC can also be utilized as a cathodic catalyst in Zn-CO_(2) battery,exhibiting high CO selectivity in the discharge process and excellent stability.This work paves a pathway to rational design of highly efficient electrocatalysts with 3D hierarchically ordered micro-macroporous architecture for CO_(2)RR towards industrial production and commercial applications.
