The Sabatier principle has been widely used for designing electrocatalysts for energy conversion applications,but it is rarely mentioned in the research of cathode catalyst of Li-CO_(2) batteries.In our work,the"...The Sabatier principle has been widely used for designing electrocatalysts for energy conversion applications,but it is rarely mentioned in the research of cathode catalyst of Li-CO_(2) batteries.In our work,the"volcanic"relationship between the catalytic activity and the adsorption energy of the catalyst to the intermediates is first demonstrated based on the first-principles calculation,which meets the Sabatier principle and can be used to design the cathode catalysts.The increases in the number of nitrogenvacancy in WN shift the d-band center and increase the interaction with the reactants.The catalytic activity increases first and then decreases with the increase of adsorption energy,which was proved in the experiment.The optimal catalyst for moderate adsorption of intermediate makes the thin LiaCO_(3) distribute evenly.It exhibits a median voltage difference of 0.68 V and an energy efficiency of 84.33%at20μA cm^(-2)with a limited capacity of 200μA h cm^(-2).展开更多
The main idea of this paper is what the resource of the serious error of the widely popular Chemical Reaction Mode catalysis Mechanism-CRMM is. The wrong definition of “catalysis, catalyst” by the catalytic academia...The main idea of this paper is what the resource of the serious error of the widely popular Chemical Reaction Mode catalysis Mechanism-CRMM is. The wrong definition of “catalysis, catalyst” by the catalytic academia boss leads to the wrong interpretation of “catalysis, catalyst” by linguists (Dictionary). The interpretation of “catalysis, catalyst” in a dictionary is misleading. The most fundamental reason for this error is that catalysis experts always believe that catalysts participate in chemical reactions. The result will appear as a series of impossible events. Such as catalysis cyclic reaction, opinions vary intermedium, catalysts repeated decomposition—formation, oxidation-reduction or life and death (enzyme), Sabatier’s principle and Boudart’s principle. The wrong theory leads the research and application of catalysts to the bottomless abyss, and industrial production suffers great losses. Electron Orbital Deformation-Recovere cyclic catalysis Mechanism-EODRM or Electron Cyclic Donate-Adopt catalysis Mechanism-ECDAM shows that the catalytic phenomenon is a physical phenomenon, not a chemical phenomenon, the catalyst does not participate in chemical reactions, only contact is the electron donate-adopt cycle, is the electron orbital deformation recovery cycle Chinese and foreign scholars should change the interpretation on the “catalysis, catalyst”, or add two new words: “contact and contactor”, it is to give up “catalysis, catalyst” altogether.展开更多
To improve the working and living environment of submarine crews, an integrated system of CO2 removal and O2 regeneration was designed to work under experimental conditions for 50 people in a submarine cabin during pr...To improve the working and living environment of submarine crews, an integrated system of CO2 removal and O2 regeneration was designed to work under experimental conditions for 50 people in a submarine cabin during prolonged voyages. The integrated system comprises a solid amine water desorption （SAWD） unit for CO2 collection and concentration, a Sabatier reactor for CO2 reduction and a solid polymer electrolyte （SPE） unit for O2 regeneration by electrolysis. The performances of the SAWD-Sabatier-SPE integrated system were investigated. The experimental results from the SAWD unit showed that the average CO2 concentration in the CO2 storage tank was more than 96% and the outlet CO2 concentration was nearly zero in the first 45 min, and less than 1/10 of inlet CO2 after 60 min when input CO2 was 0.5% （1000 L）. About 950 L of CO2 was recovered with a recovery rate of 92%-97%. The output CO2 concentration was less than 0.2%, which showed that the adsorption-desorption performance of this unit was excellent. In the CO2 reduction unit we investigated mainly the start-up and reaction performance of the Sabatier reactor. The start-up time of the Sabatier reactor was 6, 8 and 10 rain when the start-up temperature was 187.3, 179.5 and 168 ℃, respectively. The product water was colorless, transparent, and had a pH of 6.9-7.5, and an electrical conductivity of 80μs/cm. The sum of the concentration of metal ions （Ru^3＋, Al^3＋, Pb^2＋） was 0.028% and that of nonmetal ions （Cl^-, SO4^2-） was 0.05%. In the O2 regeneration unit, the O2 generation rate was 0.48 m^3/d and the quantity was 2400 L, sufficient to meet the submariners＇ basic oxygen demands. These results may be useful as a basis for establishing CO2-1evel limits and O2 regeneration systems in submarines or similar enclosed compartments during prolonged voyages.展开更多
The exploitation of competent electrocatalysts is a key issue of the broad application of many promising electrochemical processes,including the hydrogen evolution reaction(HER),the oxygen evolution reaction(OER),the ...The exploitation of competent electrocatalysts is a key issue of the broad application of many promising electrochemical processes,including the hydrogen evolution reaction(HER),the oxygen evolution reaction(OER),the oxygen reduction reaction(ORR),the CO_(2) reduction reaction(CO_(2)RR)and the nitrogen reduction reaction(NRR).The traditional searches for good electrocatalysts rely on the trial-and-error approaches,which are typically tedious and inefficient.In the past decades,some fundamental principles,activity descriptors and catalytic mechanisms have been established to accelerate the discovery of advanced electrocatalysts.Hence,it is time to summarize these theory-related research advances that unravel the structure-performance relationships and enables predictive ability in electrocatalysis studies.In this review,we summarize some basic aspects of catalytic theories that are commonly used in the design of electrocatalysts(e.g.,Sabatier principle,d-band theory,adsorption-energy scaling relation,activity descriptors)and their relevance.Then,we briefly introduced the fundamental mechanisms and central challenges of HER,OER,ORR,CO_(2)RR and NRR electrocatalysts,and highlight the theory-based efforts used to address the challenges facing these electrocatalysis processes.Finally,we propose the key challenges and opportunities of theory-driven electrocatalysis on their future.展开更多
In the original publication,the year mentioned in the references 1 and 4 of the document have two date errors.The first reference is 2021 and not 2020:Adji BI,Akaffou SD,Kouassi KH,Houphouet YP,Duminil J,Sabatier S(20...In the original publication,the year mentioned in the references 1 and 4 of the document have two date errors.The first reference is 2021 and not 2020:Adji BI,Akaffou SD,Kouassi KH,Houphouet YP,Duminil J,Sabatier S(2021)Bioclimate infl uence on seed germination and seedling morphology parameters in Pterocarpus erinaceus Poir.,1804(Fabaceae).International Journal of Environment,Agriculture and Biotechnology 6(3):2456–1878.展开更多
Efficient electrocatalytic rupture of energy-rich molecules(H_(2)and O_(2))is a green approach for gener-ating clean energy for modern societies.In this context,porphyry-type molecular electrocatalysts act intelligent...Efficient electrocatalytic rupture of energy-rich molecules(H_(2)and O_(2))is a green approach for gener-ating clean energy for modern societies.In this context,porphyry-type molecular electrocatalysts act intelligently toward oxygen reduction reaction(ORR),a fundamental process in fuel cells,due to their redox-rich chemistry,which involves core metal ions and macrocyclic ligands.The concerned scientific community has tried many times to correlate the ORR intermediates with their formation kinetics and simplify the associated multi H+/e-stages during the ORR process,constructing several volcano plots be-tween catalytic Tafel data,turnover frequencies,and overpotentials for many electrocatalysts.Despite the fact that many review articles on molecular electrocatalysts for ORR have been published,understanding the strategic implications and molecular catalyst intelligence towards homogenous ORR has been poorly explored.This review examined the relationships between volcano plots of current vs.thermodynamic parameters and the Sabatier principle in order to explain the intelligence of molecular electrocatalysts and approaches for their creation,as well as the difficulties and potential prospects of molecular electro-catalysts.These facts distinguish this review from previously published articles and will pique the scien-tific community’s interest in avoiding trial-and-error procedures for catalyst creation while also allowing for more exact evaluations of the molecular catalyst’s performance.展开更多
基金supported by the National Natural Science Foundation of China (51972225)。
文摘The Sabatier principle has been widely used for designing electrocatalysts for energy conversion applications,but it is rarely mentioned in the research of cathode catalyst of Li-CO_(2) batteries.In our work,the"volcanic"relationship between the catalytic activity and the adsorption energy of the catalyst to the intermediates is first demonstrated based on the first-principles calculation,which meets the Sabatier principle and can be used to design the cathode catalysts.The increases in the number of nitrogenvacancy in WN shift the d-band center and increase the interaction with the reactants.The catalytic activity increases first and then decreases with the increase of adsorption energy,which was proved in the experiment.The optimal catalyst for moderate adsorption of intermediate makes the thin LiaCO_(3) distribute evenly.It exhibits a median voltage difference of 0.68 V and an energy efficiency of 84.33%at20μA cm^(-2)with a limited capacity of 200μA h cm^(-2).
文摘The main idea of this paper is what the resource of the serious error of the widely popular Chemical Reaction Mode catalysis Mechanism-CRMM is. The wrong definition of “catalysis, catalyst” by the catalytic academia boss leads to the wrong interpretation of “catalysis, catalyst” by linguists (Dictionary). The interpretation of “catalysis, catalyst” in a dictionary is misleading. The most fundamental reason for this error is that catalysis experts always believe that catalysts participate in chemical reactions. The result will appear as a series of impossible events. Such as catalysis cyclic reaction, opinions vary intermedium, catalysts repeated decomposition—formation, oxidation-reduction or life and death (enzyme), Sabatier’s principle and Boudart’s principle. The wrong theory leads the research and application of catalysts to the bottomless abyss, and industrial production suffers great losses. Electron Orbital Deformation-Recovere cyclic catalysis Mechanism-EODRM or Electron Cyclic Donate-Adopt catalysis Mechanism-ECDAM shows that the catalytic phenomenon is a physical phenomenon, not a chemical phenomenon, the catalyst does not participate in chemical reactions, only contact is the electron donate-adopt cycle, is the electron orbital deformation recovery cycle Chinese and foreign scholars should change the interpretation on the “catalysis, catalyst”, or add two new words: “contact and contactor”, it is to give up “catalysis, catalyst” altogether.
基金supported by the National Natural Science Foundation of China (No. 50908062)the State Key Lab of Urban Water Resource and Environment (No. HIT-QAK200808)the Heilongjiang Natural Science Foundation (No. E2007-04), China
文摘To improve the working and living environment of submarine crews, an integrated system of CO2 removal and O2 regeneration was designed to work under experimental conditions for 50 people in a submarine cabin during prolonged voyages. The integrated system comprises a solid amine water desorption （SAWD） unit for CO2 collection and concentration, a Sabatier reactor for CO2 reduction and a solid polymer electrolyte （SPE） unit for O2 regeneration by electrolysis. The performances of the SAWD-Sabatier-SPE integrated system were investigated. The experimental results from the SAWD unit showed that the average CO2 concentration in the CO2 storage tank was more than 96% and the outlet CO2 concentration was nearly zero in the first 45 min, and less than 1/10 of inlet CO2 after 60 min when input CO2 was 0.5% （1000 L）. About 950 L of CO2 was recovered with a recovery rate of 92%-97%. The output CO2 concentration was less than 0.2%, which showed that the adsorption-desorption performance of this unit was excellent. In the CO2 reduction unit we investigated mainly the start-up and reaction performance of the Sabatier reactor. The start-up time of the Sabatier reactor was 6, 8 and 10 rain when the start-up temperature was 187.3, 179.5 and 168 ℃, respectively. The product water was colorless, transparent, and had a pH of 6.9-7.5, and an electrical conductivity of 80μs/cm. The sum of the concentration of metal ions （Ru^3＋, Al^3＋, Pb^2＋） was 0.028% and that of nonmetal ions （Cl^-, SO4^2-） was 0.05%. In the O2 regeneration unit, the O2 generation rate was 0.48 m^3/d and the quantity was 2400 L, sufficient to meet the submariners＇ basic oxygen demands. These results may be useful as a basis for establishing CO2-1evel limits and O2 regeneration systems in submarines or similar enclosed compartments during prolonged voyages.
文摘The exploitation of competent electrocatalysts is a key issue of the broad application of many promising electrochemical processes,including the hydrogen evolution reaction(HER),the oxygen evolution reaction(OER),the oxygen reduction reaction(ORR),the CO_(2) reduction reaction(CO_(2)RR)and the nitrogen reduction reaction(NRR).The traditional searches for good electrocatalysts rely on the trial-and-error approaches,which are typically tedious and inefficient.In the past decades,some fundamental principles,activity descriptors and catalytic mechanisms have been established to accelerate the discovery of advanced electrocatalysts.Hence,it is time to summarize these theory-related research advances that unravel the structure-performance relationships and enables predictive ability in electrocatalysis studies.In this review,we summarize some basic aspects of catalytic theories that are commonly used in the design of electrocatalysts(e.g.,Sabatier principle,d-band theory,adsorption-energy scaling relation,activity descriptors)and their relevance.Then,we briefly introduced the fundamental mechanisms and central challenges of HER,OER,ORR,CO_(2)RR and NRR electrocatalysts,and highlight the theory-based efforts used to address the challenges facing these electrocatalysis processes.Finally,we propose the key challenges and opportunities of theory-driven electrocatalysis on their future.
文摘In the original publication,the year mentioned in the references 1 and 4 of the document have two date errors.The first reference is 2021 and not 2020:Adji BI,Akaffou SD,Kouassi KH,Houphouet YP,Duminil J,Sabatier S(2021)Bioclimate infl uence on seed germination and seedling morphology parameters in Pterocarpus erinaceus Poir.,1804(Fabaceae).International Journal of Environment,Agriculture and Biotechnology 6(3):2456–1878.
基金funding this work through large group Research Project under grant number RGP2/172/44.
文摘Efficient electrocatalytic rupture of energy-rich molecules(H_(2)and O_(2))is a green approach for gener-ating clean energy for modern societies.In this context,porphyry-type molecular electrocatalysts act intelligently toward oxygen reduction reaction(ORR),a fundamental process in fuel cells,due to their redox-rich chemistry,which involves core metal ions and macrocyclic ligands.The concerned scientific community has tried many times to correlate the ORR intermediates with their formation kinetics and simplify the associated multi H+/e-stages during the ORR process,constructing several volcano plots be-tween catalytic Tafel data,turnover frequencies,and overpotentials for many electrocatalysts.Despite the fact that many review articles on molecular electrocatalysts for ORR have been published,understanding the strategic implications and molecular catalyst intelligence towards homogenous ORR has been poorly explored.This review examined the relationships between volcano plots of current vs.thermodynamic parameters and the Sabatier principle in order to explain the intelligence of molecular electrocatalysts and approaches for their creation,as well as the difficulties and potential prospects of molecular electro-catalysts.These facts distinguish this review from previously published articles and will pique the scien-tific community’s interest in avoiding trial-and-error procedures for catalyst creation while also allowing for more exact evaluations of the molecular catalyst’s performance.
