Electrochemical reduction of CO_(2)(CO_(2)RR)has become a research hot spot in recent years in the context of carbon neutrality.HCOOH is one of the most promising products obtained by electrochemical reduction of CO_(...Electrochemical reduction of CO_(2)(CO_(2)RR)has become a research hot spot in recent years in the context of carbon neutrality.HCOOH is one of the most promising products obtained by electrochemical reduction of CO_(2) due to its high energy value as estimated by market price per energy unit and wide application in chemical industry.Biomass is the most abundant renewable resource in the natural world.Coupling biomass oxidative conversion with CO_(2)RR driven by renewable electricity would well achieve carbon negativity.In this work,we comprehensively reviewed the current research progress on CO_(2)RR to produce HCOOH and coupled system for conversion of biomass and its derivatives to produce value-added products.Sn-and Bi-based electrocatalysts are discussed for CO_(2)RR with regards to the structure of the catalyst and reaction mechanisms.Electro-oxidation reactions of biomass derived sugars,alcohols,furan aldehydes and even polymeric components of lignocellulose were reviewed as alternatives to replace oxygen evolution reaction(OER)in the conventional electrolysis process.It was recommended that to further improve the efficiency of the coupled system,future work should be focused on the development of more efficient and stable catalysts,careful design of the electrolytic cells for improving the mass transfer and development of environment-friendly processes for recovering the formed formate and biomass oxidation products.展开更多
Electrochemical co-reduction of nitrate(NO_(3)^(-))and carbon dioxide(CO_(2))has been widely regarded as a promising route to produce urea under ambient conditions,however the yield rate of urea has remained limited.H...Electrochemical co-reduction of nitrate(NO_(3)^(-))and carbon dioxide(CO_(2))has been widely regarded as a promising route to produce urea under ambient conditions,however the yield rate of urea has remained limited.Here,we report an atomically ordered intermetallic pallium-zinc(PdZn)electrocatalyst comprising a high density of PdZn pairs for boosting urea electrosynthesis.It is found that Pd and Zn are responsible for the adsorption and activation of NO_(3)^(-)and CO_(2),respectively,and thus the co-adsorption and co-activation NO_(3)^(-)and CO_(2) are achieved in ordered PdZn pairs.More importantly,the ordered and well-defined PdZn pairs provide a dual-site geometric structure conducive to the key C-N coupling with a low kinetical barrier,as demonstrated on both operando measurements and theoretical calculations.Consequently,the PdZn electrocatalyst displays excellent performance for the co-reduction to generate urea with a maximum urea Faradaic efficiency of 62.78%and a urea yield rate of 1274.42μg mg^(-1) h^(-1),and the latter is 1.5-fold larger than disordered pairs in PdZn alloys.This work paves new pathways to boost urea electrosynthesis via constructing ordered dual-metal pairs.展开更多
Electrocatalytic reduction of CO_(2) converts intermittent renewable electricity into value-added liquid products with an enticing prospect,but its practical application is hampered due to the lack of high-performance...Electrocatalytic reduction of CO_(2) converts intermittent renewable electricity into value-added liquid products with an enticing prospect,but its practical application is hampered due to the lack of high-performance electrocatalysts.Herein,we elaborately design and develop strongly coupled nanosheets composed of Ag nanoparticles and Sn-SnO_(2) grains,designated as Ag/Sn-SnO_(2) nanosheets(NSs),which possess optimized electronic structure,high electrical conductivity,and more accessible sites.As a result,such a catalyst exhibits unprecedented catalytic performance toward CO_(2)-to-formate conversion with near-unity faradaic efficiency(≥90%),ultrahigh partial current density(2,000 mA cm^(−2)),and superior long-term stability(200 mA cm^(−2),200 h),surpassing the reported catalysts of CO_(2) electroreduction to formate.Additionally,in situ attenuated total reflection-infrared spectra combined with theoretical calculations revealed that electron-enriched Sn sites on Ag/Sn-SnO_(2)NSs not only promote the formation of*OCHO and alleviate the energy barriers of*OCHO to*HCOOH,but also impede the desorption of H*.Notably,the Ag/Sn-SnO_(2)NSs as the cathode in a membrane electrode assembly with porous solid electrolyte layer reactor can continuously produce~0.12 M pure HCOOH solution at 100 mA cm^(−2)over 200 h.This work may inspire further development of advanced electrocatalysts and innovative device systems for promoting practical application of producing liquid fuels from CO_(2).展开更多
With the advent of flexible/wearable electronic devices,flexible lithium-ion batteries(LIBs)have attracted significant attention as optimal power source candidates.Flexible LIBs with good flexibility,mechanical stabil...With the advent of flexible/wearable electronic devices,flexible lithium-ion batteries(LIBs)have attracted significant attention as optimal power source candidates.Flexible LIBs with good flexibility,mechanical stability,and high energy density are still an enormous challenge.In recent years,many complex and diverse design methods for flexible LIBs have been reported.The design and evaluation of ideal flexible LIBs must take into consideration both mechanical and electrochemical factors.In this review,the recent progress and challenges of flexible LIBs are reviewed from a mechano-electrochemical perspective.The recent progress in flexible LIB design is addressed concerning flexible material and configuration design.The mechanical and electrochemical evaluations of flexible LIBs are also summarized.Furthermore,mechano-electrochemical perspectives for the future direction of flexible LIBs are also discussed.Finally,the relationship between mechanical loading and the electrode process is analyzed from a mechano-electrochemical perspective.The evaluation of flexible LIBs should be based on mechano-electrochemical processes.Reviews and perspectives are of great significance to the design and practicality of flexible LIBs,which is contributed to bridging the gap between laboratory exploration and practical applications.展开更多
In this research, metabolic fixation of CO2 by growing cells of C. acetobutylicum cultivated with electrochemical reducing power was tested on the basis of the metabolites production and genes expression. In cyclic vo...In this research, metabolic fixation of CO2 by growing cells of C. acetobutylicum cultivated with electrochemical reducing power was tested on the basis of the metabolites production and genes expression. In cyclic voltammetry, electrochemical oxidation and reduction reaction of neutral red (NR) immobilized in intact cells of C. acetobutylicum was stationarily repeated like the soluble one in the condition without CO2 but the electrochemical reduction reaction was selectively increased by addition of CO2. In electrochemical bioreactor, the modified graphite felt cathode with NR (NR-cathode) induced C. acetobutylicum to generate acetate, propionate, and butyrate from CO2 in defined medium. When H2 and CO2 were used as an electron donor and an electron acceptor, respectively, C. acetobutylicum also produced the same metabolites in a defined medium. C. acetobutylicum was not grown in the defined medium without substituted electron donors (H2 or electrochemical reducing power). C. acetobutylicum cultivated with electrochemical reducing power produced more butyrate than acetate in complex medium but produced more acetate than butyrate in defined medium. The genes of encoding the enzymes catalyzing acetyl-CoA in C. acetobutylicum electrochemically cultivated in defined medium than conventionally cultivated in complex medium. These results are a clue that C. acetobutylicum may metabolically convert CO2 to metabolites and produce free energy from the electrochemical reducing power.展开更多
The efficient utilization of carbon dioxide(CO_(2))as a resource,comprises three key processes:CO_(2)capture,catalytic conversion and product purification.Using the renewable electricity to drive these processes provi...The efficient utilization of carbon dioxide(CO_(2))as a resource,comprises three key processes:CO_(2)capture,catalytic conversion and product purification.Using the renewable electricity to drive these processes provides a promising pathway for mitigating the ever-increasing atmospheric CO_(2)concentration whilst simultaneously addressing the growing energy demand.Although each of the three individual processes has been extensively investigated during the past decade,the rapid and economically viable reduction of CO_(2)emissions still calls for the development of an integrated electrochemical system driven by the renewable electricity to achieve carbon neutrality.Herein,we report a systematic protocol to bridge the three individual CO_(2)utilization processes into one coupled electrochemical system:a bipolar membrane electrodialysis(BPMED)cell generating alkaline and acidic solutions for the capture and recovery of CO_(2),a flow cell with an Ag gas diffusion electrode(GDE)for the selective electrocatalytic reduction of the recovered CO_(2),and an alkaline solution container for the purification of the gaseous products and recycle of the unreacted CO_(2).Consequently,the coupled electrochemical system successfully captured CO_(2)from the simulated flue gas and converted it into a pure syngas stream.展开更多
The corrosion behaviors of copper and copper/titanium galvanic couple （GC） in seawater were studied by electrochemical impedance spectroscopy （EIS） and electrochemical noise （EN） techniques in conjunction with s...The corrosion behaviors of copper and copper/titanium galvanic couple （GC） in seawater were studied by electrochemical impedance spectroscopy （EIS） and electrochemical noise （EN） techniques in conjunction with scanning electron microscopy （SEM） method. The results show that the corrosion process of copper in seawater can be divided into two stages, in which corrosion resistance and SE show the same evolution trend of initial increase and subsequent decrease, while SG changes oppositely. However, the ensemble corrosion process of copper/titanium GC in seawater includes three stages, in which corrosion resistance and SE show the evolution features of initial decrease with a subsequently increase, and the final decrease again;while SG changes oppositely. The potential difference between copper and titanium in their galvanic couple can accelerate the initiation of pitting corrosion of copper, and both the minimum and maximum corrosion potentials of copper/titanium GC are much more positive than those of pure copper.展开更多
The synthesis and modification of peptides occupy a unique position in the field of drug development,and the functionalization of amino acids is a valuable strategy as an alternative to peptide modification.Currently,...The synthesis and modification of peptides occupy a unique position in the field of drug development,and the functionalization of amino acids is a valuable strategy as an alternative to peptide modification.Currently,the development of tyrosine(Tyr)as a target amino acid is a major challenge in the field of chemistry.Herein,we report an electrochemical radical coupling reaction of labeling tyrosine-containing active drugs and peptides with thiocarbamate derivatives for the first time.This tri-component,onepot reaction can be performed smoothly under simple,gentle,and clean electrochemical conditions and is suitable for the functionalization of various Tyr-containing drug molecular derivatives and peptides.展开更多
基金supported by the National Key R&D Program of China(2022YFA2105900)the National Natural Science Foundation of China(No.22178197)。
文摘Electrochemical reduction of CO_(2)(CO_(2)RR)has become a research hot spot in recent years in the context of carbon neutrality.HCOOH is one of the most promising products obtained by electrochemical reduction of CO_(2) due to its high energy value as estimated by market price per energy unit and wide application in chemical industry.Biomass is the most abundant renewable resource in the natural world.Coupling biomass oxidative conversion with CO_(2)RR driven by renewable electricity would well achieve carbon negativity.In this work,we comprehensively reviewed the current research progress on CO_(2)RR to produce HCOOH and coupled system for conversion of biomass and its derivatives to produce value-added products.Sn-and Bi-based electrocatalysts are discussed for CO_(2)RR with regards to the structure of the catalyst and reaction mechanisms.Electro-oxidation reactions of biomass derived sugars,alcohols,furan aldehydes and even polymeric components of lignocellulose were reviewed as alternatives to replace oxygen evolution reaction(OER)in the conventional electrolysis process.It was recommended that to further improve the efficiency of the coupled system,future work should be focused on the development of more efficient and stable catalysts,careful design of the electrolytic cells for improving the mass transfer and development of environment-friendly processes for recovering the formed formate and biomass oxidation products.
基金supported by the National Natural Science Foundation of China(22379100,U21A20312)the Shenzhen Science and Technology Program(Grant No.20231121200418001)+1 种基金the Guangdong Basic and Applied Basic Research Foundation(2022B1515120084)the Key Project of Department of Education of Guangdong Province(2023ZDZX3020)。
文摘Electrochemical co-reduction of nitrate(NO_(3)^(-))and carbon dioxide(CO_(2))has been widely regarded as a promising route to produce urea under ambient conditions,however the yield rate of urea has remained limited.Here,we report an atomically ordered intermetallic pallium-zinc(PdZn)electrocatalyst comprising a high density of PdZn pairs for boosting urea electrosynthesis.It is found that Pd and Zn are responsible for the adsorption and activation of NO_(3)^(-)and CO_(2),respectively,and thus the co-adsorption and co-activation NO_(3)^(-)and CO_(2) are achieved in ordered PdZn pairs.More importantly,the ordered and well-defined PdZn pairs provide a dual-site geometric structure conducive to the key C-N coupling with a low kinetical barrier,as demonstrated on both operando measurements and theoretical calculations.Consequently,the PdZn electrocatalyst displays excellent performance for the co-reduction to generate urea with a maximum urea Faradaic efficiency of 62.78%and a urea yield rate of 1274.42μg mg^(-1) h^(-1),and the latter is 1.5-fold larger than disordered pairs in PdZn alloys.This work paves new pathways to boost urea electrosynthesis via constructing ordered dual-metal pairs.
基金the National Science Fund for Distinguished Young Scholars(Grant No.52125103)the National Natural Science Foundation of China(Grant Nos.52301232,52071041,12074048,and 12147102)China Postdoctoral Science Foundation(Grant No.2022M720552).
文摘Electrocatalytic reduction of CO_(2) converts intermittent renewable electricity into value-added liquid products with an enticing prospect,but its practical application is hampered due to the lack of high-performance electrocatalysts.Herein,we elaborately design and develop strongly coupled nanosheets composed of Ag nanoparticles and Sn-SnO_(2) grains,designated as Ag/Sn-SnO_(2) nanosheets(NSs),which possess optimized electronic structure,high electrical conductivity,and more accessible sites.As a result,such a catalyst exhibits unprecedented catalytic performance toward CO_(2)-to-formate conversion with near-unity faradaic efficiency(≥90%),ultrahigh partial current density(2,000 mA cm^(−2)),and superior long-term stability(200 mA cm^(−2),200 h),surpassing the reported catalysts of CO_(2) electroreduction to formate.Additionally,in situ attenuated total reflection-infrared spectra combined with theoretical calculations revealed that electron-enriched Sn sites on Ag/Sn-SnO_(2)NSs not only promote the formation of*OCHO and alleviate the energy barriers of*OCHO to*HCOOH,but also impede the desorption of H*.Notably,the Ag/Sn-SnO_(2)NSs as the cathode in a membrane electrode assembly with porous solid electrolyte layer reactor can continuously produce~0.12 M pure HCOOH solution at 100 mA cm^(−2)over 200 h.This work may inspire further development of advanced electrocatalysts and innovative device systems for promoting practical application of producing liquid fuels from CO_(2).
基金supported by National Natural Science Foundation of China(No.52074036)Technology Innovation Program of Beijing Institute of Technology(No.2019CX01021)BIT Teli Young Fellow。
文摘With the advent of flexible/wearable electronic devices,flexible lithium-ion batteries(LIBs)have attracted significant attention as optimal power source candidates.Flexible LIBs with good flexibility,mechanical stability,and high energy density are still an enormous challenge.In recent years,many complex and diverse design methods for flexible LIBs have been reported.The design and evaluation of ideal flexible LIBs must take into consideration both mechanical and electrochemical factors.In this review,the recent progress and challenges of flexible LIBs are reviewed from a mechano-electrochemical perspective.The recent progress in flexible LIB design is addressed concerning flexible material and configuration design.The mechanical and electrochemical evaluations of flexible LIBs are also summarized.Furthermore,mechano-electrochemical perspectives for the future direction of flexible LIBs are also discussed.Finally,the relationship between mechanical loading and the electrode process is analyzed from a mechano-electrochemical perspective.The evaluation of flexible LIBs should be based on mechano-electrochemical processes.Reviews and perspectives are of great significance to the design and practicality of flexible LIBs,which is contributed to bridging the gap between laboratory exploration and practical applications.
文摘In this research, metabolic fixation of CO2 by growing cells of C. acetobutylicum cultivated with electrochemical reducing power was tested on the basis of the metabolites production and genes expression. In cyclic voltammetry, electrochemical oxidation and reduction reaction of neutral red (NR) immobilized in intact cells of C. acetobutylicum was stationarily repeated like the soluble one in the condition without CO2 but the electrochemical reduction reaction was selectively increased by addition of CO2. In electrochemical bioreactor, the modified graphite felt cathode with NR (NR-cathode) induced C. acetobutylicum to generate acetate, propionate, and butyrate from CO2 in defined medium. When H2 and CO2 were used as an electron donor and an electron acceptor, respectively, C. acetobutylicum also produced the same metabolites in a defined medium. C. acetobutylicum was not grown in the defined medium without substituted electron donors (H2 or electrochemical reducing power). C. acetobutylicum cultivated with electrochemical reducing power produced more butyrate than acetate in complex medium but produced more acetate than butyrate in defined medium. The genes of encoding the enzymes catalyzing acetyl-CoA in C. acetobutylicum electrochemically cultivated in defined medium than conventionally cultivated in complex medium. These results are a clue that C. acetobutylicum may metabolically convert CO2 to metabolites and produce free energy from the electrochemical reducing power.
基金J.L.acknowledges the funding support from the National Key Research and Development Program of China(Grant No.2019YFE0123400 and 2022YFE0114800)the Tianjin Distinguished Young Scholars Fund(Grant No.20JCJQJC00260).
文摘The efficient utilization of carbon dioxide(CO_(2))as a resource,comprises three key processes:CO_(2)capture,catalytic conversion and product purification.Using the renewable electricity to drive these processes provides a promising pathway for mitigating the ever-increasing atmospheric CO_(2)concentration whilst simultaneously addressing the growing energy demand.Although each of the three individual processes has been extensively investigated during the past decade,the rapid and economically viable reduction of CO_(2)emissions still calls for the development of an integrated electrochemical system driven by the renewable electricity to achieve carbon neutrality.Herein,we report a systematic protocol to bridge the three individual CO_(2)utilization processes into one coupled electrochemical system:a bipolar membrane electrodialysis(BPMED)cell generating alkaline and acidic solutions for the capture and recovery of CO_(2),a flow cell with an Ag gas diffusion electrode(GDE)for the selective electrocatalytic reduction of the recovered CO_(2),and an alkaline solution container for the purification of the gaseous products and recycle of the unreacted CO_(2).Consequently,the coupled electrochemical system successfully captured CO_(2)from the simulated flue gas and converted it into a pure syngas stream.
基金Projects(21073162,51131005)supported by the National Natural Science Foundation of ChinaProject(Y4100206)supported by the Science and Technology Bureau of Jiaxing Municipality and Zhejiang Provincial Natural Science Foundation of China
文摘The corrosion behaviors of copper and copper/titanium galvanic couple （GC） in seawater were studied by electrochemical impedance spectroscopy （EIS） and electrochemical noise （EN） techniques in conjunction with scanning electron microscopy （SEM） method. The results show that the corrosion process of copper in seawater can be divided into two stages, in which corrosion resistance and SE show the same evolution trend of initial increase and subsequent decrease, while SG changes oppositely. However, the ensemble corrosion process of copper/titanium GC in seawater includes three stages, in which corrosion resistance and SE show the evolution features of initial decrease with a subsequently increase, and the final decrease again;while SG changes oppositely. The potential difference between copper and titanium in their galvanic couple can accelerate the initiation of pitting corrosion of copper, and both the minimum and maximum corrosion potentials of copper/titanium GC are much more positive than those of pure copper.
基金supported by the Guangxi Science and Technology Base and Talent Project(High level Innovative Talents and Team Training)(Guike AD23026094)the Guangxi Natural Science Foundation of China(2021GXNSFFA220005)+1 种基金the National Natural Science Foundation of China(22161008,22061003)the Innovation and Entrepreneurship Training Programme for University Students(202310602013)。
文摘The synthesis and modification of peptides occupy a unique position in the field of drug development,and the functionalization of amino acids is a valuable strategy as an alternative to peptide modification.Currently,the development of tyrosine(Tyr)as a target amino acid is a major challenge in the field of chemistry.Herein,we report an electrochemical radical coupling reaction of labeling tyrosine-containing active drugs and peptides with thiocarbamate derivatives for the first time.This tri-component,onepot reaction can be performed smoothly under simple,gentle,and clean electrochemical conditions and is suitable for the functionalization of various Tyr-containing drug molecular derivatives and peptides.
