This paper brings the comparison of performances of CO_(2)conversion by plasma and plasma-assisted catalysis based on the data collected from literature in this field,organised in an open access online database.This t...This paper brings the comparison of performances of CO_(2)conversion by plasma and plasma-assisted catalysis based on the data collected from literature in this field,organised in an open access online database.This tool is open to all users to carry out their own analyses,but also to contributors who wish to add their data to the database in order to improve the relevance of the comparisons made,and ultimately to improve the efficiency of CO_(2)conversion by plasma-catalysis.The creation of this database and database user interface is motivated by the fact that plasma-catalysis is a fast-growing field for all CO_(2)conversion processes,be it methanation,dry reforming of methane,methanolisation,or others.As a result of this rapid increase,there is a need for a set of standard procedures to rigorously compare performances of different systems.However,this is currently not possible because the fundamental mechanisms of plasma-catalysis are still too poorly understood to define these standard procedures.Fortunately however,the accumulated data within the CO_(2)plasma-catalysis community has become large enough to warrant so-called“big data”studies more familiar in the fields of medicine and the social sciences.To enable comparisons between multiple data sets and make future research more effective,this work proposes the first database on CO_(2)conversion performances by plasma-catalysis open to the whole community.This database has been initiated in the framework of a H_(2)0_(2)0 European project and is called the“PIONEER Data Base”.The database gathers a large amount of CO_(2)conversion performance data such as conversion rate,energy efficiency,and selectivity for numerous plasma sources coupled with or without a catalyst.Each data set is associated with metadata describing the gas mixture,the plasma source,the nature of the catalyst,and the form of coupling with the plasma.Beyond the database itself,a data extraction tool with direct visualisation features or advanced filtering functionalities has been developed and is available online to the public.The simple and fast visualisation of the state of the art puts new results into context,identifies literal gaps in data,and consequently points towards promising research routes.More advanced data extraction illustrates the impact that the database can have in the understanding of plasma-catalyst coupling.Lessons learned from the review of a large amount of literature during the setup of the database lead to best practice advice to increase comparability between future CO_(2)plasma-catalytic studies.Finally,the community is strongly encouraged to contribute to the database not only to increase the visibility of their data but also the relevance of the comparisons allowed by this tool.展开更多
Plasma-catalysis is considered as one of the most promising technologies for antibiotic degradation in water.In the plasma-catalytic system,one of the factors affecting the degradation effect is the performance of the...Plasma-catalysis is considered as one of the most promising technologies for antibiotic degradation in water.In the plasma-catalytic system,one of the factors affecting the degradation effect is the performance of the photocatalyst,which is usually restricted by the rapid recombination of electrons and holes as well as narrow light absorption range.In this research,a photocatalyst g-C_(3)N_(4)/TiO_(2) was prepared and coupled with gas-liquid discharge(GLD)to degrade tetracycline(TC).The performance was examined,and the degradation pathways and mechanisms were studied.Results show that a 90%degradation rate is achieved in the GLD with g-C_(3)N_(4)/TiO_(2) over a 10 min treatment.Increasing the pulse voltage is conducive to increasing the degradation rate,whereas the addition of excessive g-C_(3)N_(4)/TiO_(2) tends to precipitate agglomerates,resulting in a poor degradation efficiency.The redox properties of the g-C_(3)N_(4)/TiO_(2) surface promote the generation of oxidizing active species(H2O2,O3)in solution.Radical quenching experiments showed that·OH,hole(h^(+)),play important roles in the TC degradation by the discharge with g-C_(3)N_(4)/TiO_(2).Two potential degradation pathways were proposed based on the intermediates.The toxicity of tetracycline was reduced by treatment in the system.Furthermore,the g-C_(3)N_(4)/TiO_(2) composites exhibited excellent recoverability and stability.展开更多
The effect of temperature and hydrogen addition on undesired carbonaceous deposit formation during methane coupling was studied in DBD-plasma catalytic-wall reactors with Pd/Al2 O3, using electrical power to drive the...The effect of temperature and hydrogen addition on undesired carbonaceous deposit formation during methane coupling was studied in DBD-plasma catalytic-wall reactors with Pd/Al2 O3, using electrical power to drive the reaction.Experiments with thin catalyst layers allowed comparison of the performance of empty reactors and catalytic wall reactors without significantly influencing the plasma properties.The product distribution varies strongly in the temperature window between 25 and 200℃Minimal formation of deposits is found at an optimal temperature around 75℃ in the catalytic-wall reactors.The selectivity to deposits was c.a.10% with only 9 mg of catalyst loading instead of 45% in the blank reactor,while decreasing methane conversion only mildly.Co-feeding H2 to an empty reactor causes a similar decrease in selectivity to deposits,but in this case methane conversion also decreased significantly.Suppression of deposits formation in the catalytic-wall reactor at 75℃ is due to catalytic hydrogenation of mainly acetylene to ethylene.In the empty reactor,H2 co-feed decreases conversion but does not change the product distribution.The catalytic-wall reactors can be regenerated with H2-plasma at room temperature,which produces more added-value hydrocarbons.展开更多
The rapid accumulation of plastic waste poses severe environmental challenges.Cold plasma-driven degradation offers a promising route to convert plastic waste into high-value chemicals.In this study,a singlestage plas...The rapid accumulation of plastic waste poses severe environmental challenges.Cold plasma-driven degradation offers a promising route to convert plastic waste into high-value chemicals.In this study,a singlestage plasma reactor coupling cold plasma(dielectric barrier discharge)with Hβ zeolites was developed for polyethylene degradation under relatively mild conditions,without external thermal input or participation of noble metals.The effects of zeolite pore structure and acidity toward product distribution were investigated,revealing that Hβ-25 exhibited the highest C_(1)-C_(6) yield(76 wt%)and a space-time yield of 103.8 mmol·g_(cat)^(-1)·h^(-1) compared to other zeolite catalysts during the plasma-catalytic process.Meanwhile,it was revealed that efficient precracking initiated by plasma activation and the optimal structural compatibility between Hβ-zeolite pore channels and primary cracking products were the key factors enabling the selective conversion of polyethylene into C_(1)-C_(6) hydrocarbons.Additionally,metal incorporation significantly enhanced C-H bond cleavage compared to Hβ-25 support.Especially,10Ni/Hβ-25 exhibited the highest hydrogen yield(7.87 mmol·g_(plastic)^(-1))under plasmaassisted mode,markedly surpassing its yield under thermal-cracking conditions,demonstrating the significant potential of plasma-catalytic degradation for hydrogen production from polyethylene.展开更多
基金funding from the European Union’s Horizon 2020 research and innovation programme under the Marie Sklodowska-Curie grant agreement No.813393partially funded by the Portuguese FCT-Funda??o para a Ciência e a Tecnologia,under projects UIDB/50010/2020,UIDP/50010/2020 and PTDC/FIS-PLA/1616/2021。
文摘This paper brings the comparison of performances of CO_(2)conversion by plasma and plasma-assisted catalysis based on the data collected from literature in this field,organised in an open access online database.This tool is open to all users to carry out their own analyses,but also to contributors who wish to add their data to the database in order to improve the relevance of the comparisons made,and ultimately to improve the efficiency of CO_(2)conversion by plasma-catalysis.The creation of this database and database user interface is motivated by the fact that plasma-catalysis is a fast-growing field for all CO_(2)conversion processes,be it methanation,dry reforming of methane,methanolisation,or others.As a result of this rapid increase,there is a need for a set of standard procedures to rigorously compare performances of different systems.However,this is currently not possible because the fundamental mechanisms of plasma-catalysis are still too poorly understood to define these standard procedures.Fortunately however,the accumulated data within the CO_(2)plasma-catalysis community has become large enough to warrant so-called“big data”studies more familiar in the fields of medicine and the social sciences.To enable comparisons between multiple data sets and make future research more effective,this work proposes the first database on CO_(2)conversion performances by plasma-catalysis open to the whole community.This database has been initiated in the framework of a H_(2)0_(2)0 European project and is called the“PIONEER Data Base”.The database gathers a large amount of CO_(2)conversion performance data such as conversion rate,energy efficiency,and selectivity for numerous plasma sources coupled with or without a catalyst.Each data set is associated with metadata describing the gas mixture,the plasma source,the nature of the catalyst,and the form of coupling with the plasma.Beyond the database itself,a data extraction tool with direct visualisation features or advanced filtering functionalities has been developed and is available online to the public.The simple and fast visualisation of the state of the art puts new results into context,identifies literal gaps in data,and consequently points towards promising research routes.More advanced data extraction illustrates the impact that the database can have in the understanding of plasma-catalyst coupling.Lessons learned from the review of a large amount of literature during the setup of the database lead to best practice advice to increase comparability between future CO_(2)plasma-catalytic studies.Finally,the community is strongly encouraged to contribute to the database not only to increase the visibility of their data but also the relevance of the comparisons allowed by this tool.
基金supported by National Natural Science Foundation of China(Nos.52277151 and 51907088)Innovative Talents Team Project of‘Six Talent Peaks’of Jiangsu Province(No.TD-JNHB-006).
文摘Plasma-catalysis is considered as one of the most promising technologies for antibiotic degradation in water.In the plasma-catalytic system,one of the factors affecting the degradation effect is the performance of the photocatalyst,which is usually restricted by the rapid recombination of electrons and holes as well as narrow light absorption range.In this research,a photocatalyst g-C_(3)N_(4)/TiO_(2) was prepared and coupled with gas-liquid discharge(GLD)to degrade tetracycline(TC).The performance was examined,and the degradation pathways and mechanisms were studied.Results show that a 90%degradation rate is achieved in the GLD with g-C_(3)N_(4)/TiO_(2) over a 10 min treatment.Increasing the pulse voltage is conducive to increasing the degradation rate,whereas the addition of excessive g-C_(3)N_(4)/TiO_(2) tends to precipitate agglomerates,resulting in a poor degradation efficiency.The redox properties of the g-C_(3)N_(4)/TiO_(2) surface promote the generation of oxidizing active species(H2O2,O3)in solution.Radical quenching experiments showed that·OH,hole(h^(+)),play important roles in the TC degradation by the discharge with g-C_(3)N_(4)/TiO_(2).Two potential degradation pathways were proposed based on the intermediates.The toxicity of tetracycline was reduced by treatment in the system.Furthermore,the g-C_(3)N_(4)/TiO_(2) composites exhibited excellent recoverability and stability.
基金supported by the Innovation Fund for Chemistry of NWO,grant number 731.014.303by SASOL。
文摘The effect of temperature and hydrogen addition on undesired carbonaceous deposit formation during methane coupling was studied in DBD-plasma catalytic-wall reactors with Pd/Al2 O3, using electrical power to drive the reaction.Experiments with thin catalyst layers allowed comparison of the performance of empty reactors and catalytic wall reactors without significantly influencing the plasma properties.The product distribution varies strongly in the temperature window between 25 and 200℃Minimal formation of deposits is found at an optimal temperature around 75℃ in the catalytic-wall reactors.The selectivity to deposits was c.a.10% with only 9 mg of catalyst loading instead of 45% in the blank reactor,while decreasing methane conversion only mildly.Co-feeding H2 to an empty reactor causes a similar decrease in selectivity to deposits,but in this case methane conversion also decreased significantly.Suppression of deposits formation in the catalytic-wall reactor at 75℃ is due to catalytic hydrogenation of mainly acetylene to ethylene.In the empty reactor,H2 co-feed decreases conversion but does not change the product distribution.The catalytic-wall reactors can be regenerated with H2-plasma at room temperature,which produces more added-value hydrocarbons.
基金financially supported by the National Key R&D Program of China(Grant Nos.2023YFA1506602 and 2021YFA1501102)the National Natural Science Foundation of China(Grant Nos.21932002,22276023,and 22402019)+1 种基金the Fundamental Research Funds for the Central Universities(Grant No.DUT22LAB602)the Liaoning Binhai Laboratory Project(Grant No.LBLF-202306).
文摘The rapid accumulation of plastic waste poses severe environmental challenges.Cold plasma-driven degradation offers a promising route to convert plastic waste into high-value chemicals.In this study,a singlestage plasma reactor coupling cold plasma(dielectric barrier discharge)with Hβ zeolites was developed for polyethylene degradation under relatively mild conditions,without external thermal input or participation of noble metals.The effects of zeolite pore structure and acidity toward product distribution were investigated,revealing that Hβ-25 exhibited the highest C_(1)-C_(6) yield(76 wt%)and a space-time yield of 103.8 mmol·g_(cat)^(-1)·h^(-1) compared to other zeolite catalysts during the plasma-catalytic process.Meanwhile,it was revealed that efficient precracking initiated by plasma activation and the optimal structural compatibility between Hβ-zeolite pore channels and primary cracking products were the key factors enabling the selective conversion of polyethylene into C_(1)-C_(6) hydrocarbons.Additionally,metal incorporation significantly enhanced C-H bond cleavage compared to Hβ-25 support.Especially,10Ni/Hβ-25 exhibited the highest hydrogen yield(7.87 mmol·g_(plastic)^(-1))under plasmaassisted mode,markedly surpassing its yield under thermal-cracking conditions,demonstrating the significant potential of plasma-catalytic degradation for hydrogen production from polyethylene.
