Orbital hybridization plays a crucial role in catalytic processes,yet elucidating its mechanism remains a significant challenge.Here,we have developed a strategy for the formation of Yb-C bond by unconventional p-d or...Orbital hybridization plays a crucial role in catalytic processes,yet elucidating its mechanism remains a significant challenge.Here,we have developed a strategy for the formation of Yb-C bond by unconventional p-d orbital hybridization,which induced carbon nitride modified by rare-earth metal element Yb.The optimal sample exhibits catalytic performance 11.2 times greater than that of g-C_(3)N_(4)with N vacancies(NvCN).Yb-C bond and N vacancies reduced the energy barrier and optimized the rate-determining step(*COO+*H→*CO+*OH).Additionally,the intense Yb-C interaction created a specific electrons bridge,which accelerated the transfer rate of electrons on the photocatalytic surface.Next,the CO_(2) conversion reaction mechanism was studied by in situ infrared spectroscopy and theoretical calculations,and the unconventional p-d orbital hybridization contributed to the generation of vital intermediate*CO.This study provides a theoretical basis for designing single-atom photocatalysts for the reduction of CO_(2).展开更多
The rapid expansion of the chemical and pharmaceutical industries has resulted in the introduction of various sources of micropollutants into the environment,posing threats to drinking water quality and public health....The rapid expansion of the chemical and pharmaceutical industries has resulted in the introduction of various sources of micropollutants into the environment,posing threats to drinking water quality and public health.Membrane separation technology offers a promising solution with low energy use,high-quality effluent,and operational simplicity.Here,we developed fluffy layered double hydroxides(LDH)/graphene oxide(GO)2D membranes,specifically tannic acid-mediated LDH-GO/GO-TA composite membranes(LG/GT).The integration of GO nanosheets regulated the growth of LDH,enhancing electron transfer and adsorption-driven catalytic performance.This design enabled LDH-GO to activate peroxymonosulfate(PMS)and completely degraded Rhodamine B(RhB)within 10 min.The Gaussian calculation was combined with this finding,which could explain the catalytic self-cleaning in the separation process.The TA-mediated enhancement further increased the RhB rejection of LG/GT-7.5 to 99.23%.Additionally,the needle/sheet structure significantly improved permeance to 358.28 L m^(-2) h^(-1) bar^(-1),surpassing the L/GT-7.5 performance(e.g.338.53 L m^(-2) h^(-1) bar^(-1)),indicating superior pore formation and water mass transfer.The heterostructure between GO and LDH greatly improved cycling stability,with the membrane maintaining a permeance of 282.71 L m^(-2) h^(-1) bar^(-1) and a rejection of 97.97% despite 20 cycles.This work demonstrated the potential of fluffy layered LDH 2D membranes for enhanced wastewater treatment applications.These findings suggested significant potential for practical implementation in industrial wastewater treatment processes,offering a sustainable and efficient solution to water pollution challenges.展开更多
Municipal solid waste(MSW)management has emerged as probably the most pressing issue many governments nowadays are facing.Traditionally,Waste-to-Energy(WtE)is mostly associated with incineration,but now,with the emerg...Municipal solid waste(MSW)management has emerged as probably the most pressing issue many governments nowadays are facing.Traditionally,Waste-to-Energy(WtE)is mostly associated with incineration,but now,with the emergence of the bioeconomy,it embraces a broader definition comprising any processing technique that can generate electricity/heat or produce a waste-derived fuel.Under the ambit of the circular economy many nations are looking for,additional effort must be made to be sure of acquiring the most updated information and paving a sustainable path for managing MSW in such a frame.In this regard,we have undertaken a critical review of various technologies,with their updated progress,involved in the exploitation of MSW as a renewable resource,along with the critical advantages and limitations on energy and material cycling for sustainable MSW management.Incineration,the most widely used method,is nowadays difficult to further apply due to its dubious reputation and social opposition.Meanwhile,to address the organic fraction of MSW which currently is mostly unrecycled and causes disposal issues,the biological approach presents an attractive option.The new emphasis of bioeconomy leads us to understand how environmental biotechnologies should be better connected/integrated for more sustainable MSW management.This article is concluded with advances of future prospects,which can serve as a timely reminder to encourage competent authorities/researchers to work towards further improvement of the present MSW management system.展开更多
Iron element is known to be an effective additive for accelerating the anaerobic digestion(AD)process for treating organic wastes.However,the effects of different kinds of iron additives on food waste(FW)and sewage sl...Iron element is known to be an effective additive for accelerating the anaerobic digestion(AD)process for treating organic wastes.However,the effects of different kinds of iron additives on food waste(FW)and sewage sludge of co-digestion process have not been yet investigated thoroughly.This study aimed to elucidate how different kinds of iron components affect methane production during FW and sewage sludge anaerobic co-digestion(co-AD)process and to investigate the possible mechanism of Fe amendment.Experimental results revealed that Fe amendment could effectively promote the substrate degradation and methane production,and FeCl3 amended group presented the best digestion performance,boosting the methane production from 465.9 mL to 2650.4 mL.The results of the excitation-emission matrix fluorescence spectra analysis further supported that Fe supplements facilitated the waste hydrolysis with a higher concentration of dissolved organic matters and thereby more substrates can be used for methane generation.In addition,the activity of coenzyme F420 and direct interspecies electron transfer in FeCl3 group were 5.82 and 5.89 times higher than those in the control group,respectively,indicating that electron transfer,particularly the interspecies one,was enhanced by Fe amendment.As compared to that in the control group,the increased cytochrome c concentration in Fe amended groups also proved it.Therefore,this study will provide a reference regarding Fe amendment in the co-AD process for FW and sewage sludge.展开更多
基金financially supported by the National Natural Science Foundation of China(No.52370109)Guangdong Province Scientific Research Platform Project(Nos.2023ZDZX4052,2022ZDZX4046)+3 种基金Shaoguan Science and Technology Projects(No.230616088031998)High Level Talents Introduction Project of"Pearl River Talent Plan"in Guangdong Province(No.2019CX01L308)the Support Scheme of Guangzhou for Leading Talents in Innovation and Entrepreneurship Funding(No.2016015)the Science and Technology Research Program of Chongqing Municipal Education Commission of China(No.KJZDM202400802)
文摘Orbital hybridization plays a crucial role in catalytic processes,yet elucidating its mechanism remains a significant challenge.Here,we have developed a strategy for the formation of Yb-C bond by unconventional p-d orbital hybridization,which induced carbon nitride modified by rare-earth metal element Yb.The optimal sample exhibits catalytic performance 11.2 times greater than that of g-C_(3)N_(4)with N vacancies(NvCN).Yb-C bond and N vacancies reduced the energy barrier and optimized the rate-determining step(*COO+*H→*CO+*OH).Additionally,the intense Yb-C interaction created a specific electrons bridge,which accelerated the transfer rate of electrons on the photocatalytic surface.Next,the CO_(2) conversion reaction mechanism was studied by in situ infrared spectroscopy and theoretical calculations,and the unconventional p-d orbital hybridization contributed to the generation of vital intermediate*CO.This study provides a theoretical basis for designing single-atom photocatalysts for the reduction of CO_(2).
基金supported by Jiangsu Funding Program for Excellent postdoctoral Talent(2023ZB453 and 2023ZB108)National Natural Science Foundation of China(22306075 and 22108103)Hong Kong Environment and Conservation Fund(2022-127).
文摘The rapid expansion of the chemical and pharmaceutical industries has resulted in the introduction of various sources of micropollutants into the environment,posing threats to drinking water quality and public health.Membrane separation technology offers a promising solution with low energy use,high-quality effluent,and operational simplicity.Here,we developed fluffy layered double hydroxides(LDH)/graphene oxide(GO)2D membranes,specifically tannic acid-mediated LDH-GO/GO-TA composite membranes(LG/GT).The integration of GO nanosheets regulated the growth of LDH,enhancing electron transfer and adsorption-driven catalytic performance.This design enabled LDH-GO to activate peroxymonosulfate(PMS)and completely degraded Rhodamine B(RhB)within 10 min.The Gaussian calculation was combined with this finding,which could explain the catalytic self-cleaning in the separation process.The TA-mediated enhancement further increased the RhB rejection of LG/GT-7.5 to 99.23%.Additionally,the needle/sheet structure significantly improved permeance to 358.28 L m^(-2) h^(-1) bar^(-1),surpassing the L/GT-7.5 performance(e.g.338.53 L m^(-2) h^(-1) bar^(-1)),indicating superior pore formation and water mass transfer.The heterostructure between GO and LDH greatly improved cycling stability,with the membrane maintaining a permeance of 282.71 L m^(-2) h^(-1) bar^(-1) and a rejection of 97.97% despite 20 cycles.This work demonstrated the potential of fluffy layered LDH 2D membranes for enhanced wastewater treatment applications.These findings suggested significant potential for practical implementation in industrial wastewater treatment processes,offering a sustainable and efficient solution to water pollution challenges.
文摘Municipal solid waste(MSW)management has emerged as probably the most pressing issue many governments nowadays are facing.Traditionally,Waste-to-Energy(WtE)is mostly associated with incineration,but now,with the emergence of the bioeconomy,it embraces a broader definition comprising any processing technique that can generate electricity/heat or produce a waste-derived fuel.Under the ambit of the circular economy many nations are looking for,additional effort must be made to be sure of acquiring the most updated information and paving a sustainable path for managing MSW in such a frame.In this regard,we have undertaken a critical review of various technologies,with their updated progress,involved in the exploitation of MSW as a renewable resource,along with the critical advantages and limitations on energy and material cycling for sustainable MSW management.Incineration,the most widely used method,is nowadays difficult to further apply due to its dubious reputation and social opposition.Meanwhile,to address the organic fraction of MSW which currently is mostly unrecycled and causes disposal issues,the biological approach presents an attractive option.The new emphasis of bioeconomy leads us to understand how environmental biotechnologies should be better connected/integrated for more sustainable MSW management.This article is concluded with advances of future prospects,which can serve as a timely reminder to encourage competent authorities/researchers to work towards further improvement of the present MSW management system.
基金funding provided by Hong Kong Baptist University Libraryfinancially supported by National Natural Science Foundation of China(No.51978595).
文摘Iron element is known to be an effective additive for accelerating the anaerobic digestion(AD)process for treating organic wastes.However,the effects of different kinds of iron additives on food waste(FW)and sewage sludge of co-digestion process have not been yet investigated thoroughly.This study aimed to elucidate how different kinds of iron components affect methane production during FW and sewage sludge anaerobic co-digestion(co-AD)process and to investigate the possible mechanism of Fe amendment.Experimental results revealed that Fe amendment could effectively promote the substrate degradation and methane production,and FeCl3 amended group presented the best digestion performance,boosting the methane production from 465.9 mL to 2650.4 mL.The results of the excitation-emission matrix fluorescence spectra analysis further supported that Fe supplements facilitated the waste hydrolysis with a higher concentration of dissolved organic matters and thereby more substrates can be used for methane generation.In addition,the activity of coenzyme F420 and direct interspecies electron transfer in FeCl3 group were 5.82 and 5.89 times higher than those in the control group,respectively,indicating that electron transfer,particularly the interspecies one,was enhanced by Fe amendment.As compared to that in the control group,the increased cytochrome c concentration in Fe amended groups also proved it.Therefore,this study will provide a reference regarding Fe amendment in the co-AD process for FW and sewage sludge.
