The interplay between multi-atom assembly configurations and single atoms(SAs)has been gaining attention in research.However,the effect of long-term range interactions between SAs and multi-atom assemblies on the orbi...The interplay between multi-atom assembly configurations and single atoms(SAs)has been gaining attention in research.However,the effect of long-term range interactions between SAs and multi-atom assemblies on the orbital filling characteristics has yet to be investigated.In this context,we introduced copper(Cu)doping to strengthen the interaction between cobalt(Co)nanoparticles(NPs)and Co SAs by promoting the spontaneous formation of Co-Cu alloy NPs that tends toward aggregation owing to its negative cohesive energy(-0.06454),instead of forming Cu SAs.The incorporation of Cu within the Co-Cu alloy NPs,compared to the pure Co NPs,significantly expedites the kinetics of peroxymonosulfate(PMS)oxidation processes on Co SAs.Unlike Co NPs,Co-Cu NPs facilitate electron rearrangement in the d orbitals(especially dz^(2)and dxz)near the Fermi level in Co SAs,thereby optimizing the dz^(2)-O(PMS)and dxz-O(SO_(5)^(-))orbital interaction.Eventually,the Co-Cu alloy NPs embedded in nitrogen-doped carbon(CC@CNC)catalysts rapidly eliminated 80.67% of 20 mg L^(-1)carbamazepine(CBZ)within 5 min.This performance significantly surpasses that of catalysts consisting solely of Co NPs in a similar matrix(C@CNC),which achieved a 58.99% reduction in 5 min.The quasi in situ characterization suggested that PMS acts as an electron donor and will transfer electrons to Co SAs,generating^(1)O_(2)for contaminant abatement.This study offers valuable insights into the mechanisms by which composite active sites formed through multi-atom assembly interact at the atomic orbital level to achieve high-efficiency PMS-based advanced oxidation processes at the atomic orbital level.展开更多
Biochar(BC)and nanoparticle-decorated biochar(NPs@BC)have emerged as potential high-performance function materials to facilitate simultaneous soil remediation and agricultural production.Therefore,there is an urgent n...Biochar(BC)and nanoparticle-decorated biochar(NPs@BC)have emerged as potential high-performance function materials to facilitate simultaneous soil remediation and agricultural production.Therefore,there is an urgent need to incorporate environmental sustainability and human health targets into BC and NPs@BC selection and design processes.In contrast to extensive research on the preparation,modification,and environmental application of BC to soil ecosystems,reports about the adapted framework and material selection strategy of NPs@BC under environmental and human health considerations are still limited.Nevertheless,few studies systematically explored the impact of NPs@BC on soil ecosystems,including soil biota,geochemical properties,and nutrient cycles,which are critical for largescale utilization as a multifunctional product.The main objective of this systematic literature review is to show the high degrees of contaminant removal for different heavy metals and organic pollutants,and to quantify the economic,environmental,and toxicological outcomes of NPs@BC in the context of sustainable agriculture.To address this need,in this review,we summarized synthesis techniques and characterization,and highlighted a linkage between the evolution of NPs@BC properties with the framework for sustainable NPs@BC selection and design based on environmental effects,hazards,and economic considerations.Then,research advances in contaminant remediation for heavy metals and organic pollutants of NPs@BC are minutely discussed.Eventually,NPs@BC positively acts on sustainable agriculture,which is declared.In the meantime,evaluating from the perspective of plant growth,soil characterizations as well as carbon and nitrogen cycle was conducted,which is critical for comprehending the NPs@BC environmental sustainability.Our work may develop a potential framework that can inform decision-making for the use of NPs@BC to facilitate promising environmental applications and prevent unintended consequences,and is expected to guide and boost the development of highly efficient NPs@BC for sustainable agriculture and environmental applications.展开更多
基金supported by the Ministry of Science and Technology of People’s Republic of China as a Key Technology Research and Development Program Project(2023YFC3709001 and2019YFC1804104)the Ministry of Education of People’s Republic of China as a Discipline Innovation and Intelligence Introduction Project(B17025)+3 种基金the National Natural Science Foundation of China as a Shandong Joint Fund Project(U1906222)the Tianjin Science and Technology Bureau as a Key Science and Technology Supporting Project(19YFZCSF00920)the Shiyanjia Lab(www.shiyanjia.com)for the support of experimental analysesApplied Chemistry and Engineering Institute(Nankai University)for the instrument support of ACTEM(JEM-ARM200F)。
文摘The interplay between multi-atom assembly configurations and single atoms(SAs)has been gaining attention in research.However,the effect of long-term range interactions between SAs and multi-atom assemblies on the orbital filling characteristics has yet to be investigated.In this context,we introduced copper(Cu)doping to strengthen the interaction between cobalt(Co)nanoparticles(NPs)and Co SAs by promoting the spontaneous formation of Co-Cu alloy NPs that tends toward aggregation owing to its negative cohesive energy(-0.06454),instead of forming Cu SAs.The incorporation of Cu within the Co-Cu alloy NPs,compared to the pure Co NPs,significantly expedites the kinetics of peroxymonosulfate(PMS)oxidation processes on Co SAs.Unlike Co NPs,Co-Cu NPs facilitate electron rearrangement in the d orbitals(especially dz^(2)and dxz)near the Fermi level in Co SAs,thereby optimizing the dz^(2)-O(PMS)and dxz-O(SO_(5)^(-))orbital interaction.Eventually,the Co-Cu alloy NPs embedded in nitrogen-doped carbon(CC@CNC)catalysts rapidly eliminated 80.67% of 20 mg L^(-1)carbamazepine(CBZ)within 5 min.This performance significantly surpasses that of catalysts consisting solely of Co NPs in a similar matrix(C@CNC),which achieved a 58.99% reduction in 5 min.The quasi in situ characterization suggested that PMS acts as an electron donor and will transfer electrons to Co SAs,generating^(1)O_(2)for contaminant abatement.This study offers valuable insights into the mechanisms by which composite active sites formed through multi-atom assembly interact at the atomic orbital level to achieve high-efficiency PMS-based advanced oxidation processes at the atomic orbital level.
基金National Natural Science Foundation of China(NO.42107306,U1906222)Fellowship of China Postdoctoral Science Foundation(NO.2020M680867)+1 种基金National Key Research and Development Project(NO.2019YFC1804104)Ministry of Education,People’s Republic of China as a 111 program(NO.T2017002).
文摘Biochar(BC)and nanoparticle-decorated biochar(NPs@BC)have emerged as potential high-performance function materials to facilitate simultaneous soil remediation and agricultural production.Therefore,there is an urgent need to incorporate environmental sustainability and human health targets into BC and NPs@BC selection and design processes.In contrast to extensive research on the preparation,modification,and environmental application of BC to soil ecosystems,reports about the adapted framework and material selection strategy of NPs@BC under environmental and human health considerations are still limited.Nevertheless,few studies systematically explored the impact of NPs@BC on soil ecosystems,including soil biota,geochemical properties,and nutrient cycles,which are critical for largescale utilization as a multifunctional product.The main objective of this systematic literature review is to show the high degrees of contaminant removal for different heavy metals and organic pollutants,and to quantify the economic,environmental,and toxicological outcomes of NPs@BC in the context of sustainable agriculture.To address this need,in this review,we summarized synthesis techniques and characterization,and highlighted a linkage between the evolution of NPs@BC properties with the framework for sustainable NPs@BC selection and design based on environmental effects,hazards,and economic considerations.Then,research advances in contaminant remediation for heavy metals and organic pollutants of NPs@BC are minutely discussed.Eventually,NPs@BC positively acts on sustainable agriculture,which is declared.In the meantime,evaluating from the perspective of plant growth,soil characterizations as well as carbon and nitrogen cycle was conducted,which is critical for comprehending the NPs@BC environmental sustainability.Our work may develop a potential framework that can inform decision-making for the use of NPs@BC to facilitate promising environmental applications and prevent unintended consequences,and is expected to guide and boost the development of highly efficient NPs@BC for sustainable agriculture and environmental applications.