Ethylene,one of the most widely produced building blocks in the petrochemical industry,has received intense attention.Ethylene production,using electrochemical hydrogen pump-facilitated nonoxidative dehydrogenation of...Ethylene,one of the most widely produced building blocks in the petrochemical industry,has received intense attention.Ethylene production,using electrochemical hydrogen pump-facilitated nonoxidative dehydrogenation of ethane(NDE)to ethylene,is an emerging and promising route,promoting the transformation of the ethylene industry from energy-intensive steam cracking process to new electrochemical membrane reactor technology.In this work,the NDE reaction is incorporated into a BaZr_(0.1)Ce_(0.7)Y_(0.1)Yb_(0.1)O_(3-δ)electrolyte-supported protonic ceramic fuel cell membrane reactor to co-generate electricity and ethylene,utilizing the Nb and Cu doped perovskite oxide Pr_(0.6)Sr_(0.4)Fe_(0.8)Nb_(0.1)Cu_(0.1)O_(3-δ)(PSFNCu)as anode catalytic layer.Due to the doping of Nb and Cu,PSFNCu was endowed with high reduction tolerance and rich oxygen vacancies,showing excellent NDE catalytic performance.The maximum power density of the assembled reactor reaches 200 mW cm^(-2)at 750℃,with high ethane conversion(44.9%)and ethylene selectivity(92.7%).Moreover,the nitrous oxide decomposition was first coupled in the protonic ceramic fuel cell membrane reactor to consume the permeated protons.As a result,the generation of electricity,ethylene and decomposition of nitrous oxide can be simultaneously obtained by a single reactor.Specifically,the maximum power density of the cell reaches 208 mW cm^(-2)at 750℃,with high ethane conversion(45.2%),ethylene selectivity(92.5%),and nitrous oxide conversion(19,0%).This multi-win technology is promising for not only the production of chemicals and energy but also greenhouse gas reduction.展开更多
High-concentration industrial wastewater containing N,N-dimethylacetamide(DMAc)from polymeric membrane manufacturer was degraded in Cu2O NPs/H2O2 Fenton.process.In the membrane assisted Fenton process DMAc removal rat...High-concentration industrial wastewater containing N,N-dimethylacetamide(DMAc)from polymeric membrane manufacturer was degraded in Cu2O NPs/H2O2 Fenton.process.In the membrane assisted Fenton process DMAc removal rate was up to 98%with 120 min which was increased by 23%over the batch reactor.It was found that:OH quench time was extended by 20 min and the maximum:0H productivity was notably 88.7%higher at 40 min.The degradation reaction rate constant was enhanced by 2.2 times with membrane dispersion(k=0.0349 min^-1).DMAc initial concentration(C0)and H202 flux (Jp)had major influence on mass transfer and kinetics,meanwhile,membrane pore size(rp)and length(L)also affected the Treaction rate.The intensifed radical yield,fast mass transfer and nanoparticles high activity all contributed to improve pollutant degradation eficiency.Time-resolved DMAC degradation pathway was analyzed as hydroxylation,demethylation and oxidation leading to the finai products of CO2;H20 and NO3^-(rather.than NH,from biodegradation).Continuous process was operated in the dual-membrane configuration with in situ reaction and separation.After five cycling,tests,DMAc removal was all above 95%for the initial[DMAc]0=14,000 mg/L in wastewater and stability of the catalyst and the membrane maintained weil.展开更多
CH4-CO2-O-2 reforming to syngas in a never Ba0.5Sr0.5Co0.8Fe0.2O3.delta oxygen-permeable membrane reactor using LiLaNiO/gamma-Al2O3 as catalyst was successfully reported. Excellent reaction performance was achieved wi...CH4-CO2-O-2 reforming to syngas in a never Ba0.5Sr0.5Co0.8Fe0.2O3.delta oxygen-permeable membrane reactor using LiLaNiO/gamma-Al2O3 as catalyst was successfully reported. Excellent reaction performance was achieved with around 92% methane conversion efficiency, 95% CO2 conversion rate, and nearly 8.5mL/min.cm(2) oxygen permeation flux. In contrast to the oxygen permeation model with the presence of large concentration of CO2 (under such condition the oxygen permeation flux deteriorates with time), the oxygen permeation flux is really stable under the CH4CO2-O-2 reforming condition.展开更多
基金funding from the National Key R&D Program of China(2020YFB1505603)the Natural Science Foundation of China(22075086,22138005,22141001)the Guangdong Basic and Applied Basic Research Foundation(2019A1515011512,2020A1515011157,2021A1515010172,2022A1515010980)。
文摘Ethylene,one of the most widely produced building blocks in the petrochemical industry,has received intense attention.Ethylene production,using electrochemical hydrogen pump-facilitated nonoxidative dehydrogenation of ethane(NDE)to ethylene,is an emerging and promising route,promoting the transformation of the ethylene industry from energy-intensive steam cracking process to new electrochemical membrane reactor technology.In this work,the NDE reaction is incorporated into a BaZr_(0.1)Ce_(0.7)Y_(0.1)Yb_(0.1)O_(3-δ)electrolyte-supported protonic ceramic fuel cell membrane reactor to co-generate electricity and ethylene,utilizing the Nb and Cu doped perovskite oxide Pr_(0.6)Sr_(0.4)Fe_(0.8)Nb_(0.1)Cu_(0.1)O_(3-δ)(PSFNCu)as anode catalytic layer.Due to the doping of Nb and Cu,PSFNCu was endowed with high reduction tolerance and rich oxygen vacancies,showing excellent NDE catalytic performance.The maximum power density of the assembled reactor reaches 200 mW cm^(-2)at 750℃,with high ethane conversion(44.9%)and ethylene selectivity(92.7%).Moreover,the nitrous oxide decomposition was first coupled in the protonic ceramic fuel cell membrane reactor to consume the permeated protons.As a result,the generation of electricity,ethylene and decomposition of nitrous oxide can be simultaneously obtained by a single reactor.Specifically,the maximum power density of the cell reaches 208 mW cm^(-2)at 750℃,with high ethane conversion(45.2%),ethylene selectivity(92.5%),and nitrous oxide conversion(19,0%).This multi-win technology is promising for not only the production of chemicals and energy but also greenhouse gas reduction.
基金The authors would like to acknowledge the financial support from National Natural Science Foundation of China(Grant No.21921006).
文摘High-concentration industrial wastewater containing N,N-dimethylacetamide(DMAc)from polymeric membrane manufacturer was degraded in Cu2O NPs/H2O2 Fenton.process.In the membrane assisted Fenton process DMAc removal rate was up to 98%with 120 min which was increased by 23%over the batch reactor.It was found that:OH quench time was extended by 20 min and the maximum:0H productivity was notably 88.7%higher at 40 min.The degradation reaction rate constant was enhanced by 2.2 times with membrane dispersion(k=0.0349 min^-1).DMAc initial concentration(C0)and H202 flux (Jp)had major influence on mass transfer and kinetics,meanwhile,membrane pore size(rp)and length(L)also affected the Treaction rate.The intensifed radical yield,fast mass transfer and nanoparticles high activity all contributed to improve pollutant degradation eficiency.Time-resolved DMAC degradation pathway was analyzed as hydroxylation,demethylation and oxidation leading to the finai products of CO2;H20 and NO3^-(rather.than NH,from biodegradation).Continuous process was operated in the dual-membrane configuration with in situ reaction and separation.After five cycling,tests,DMAc removal was all above 95%for the initial[DMAc]0=14,000 mg/L in wastewater and stability of the catalyst and the membrane maintained weil.
文摘CH4-CO2-O-2 reforming to syngas in a never Ba0.5Sr0.5Co0.8Fe0.2O3.delta oxygen-permeable membrane reactor using LiLaNiO/gamma-Al2O3 as catalyst was successfully reported. Excellent reaction performance was achieved with around 92% methane conversion efficiency, 95% CO2 conversion rate, and nearly 8.5mL/min.cm(2) oxygen permeation flux. In contrast to the oxygen permeation model with the presence of large concentration of CO2 (under such condition the oxygen permeation flux deteriorates with time), the oxygen permeation flux is really stable under the CH4CO2-O-2 reforming condition.