In recent years,biochar(BC)as a low-cost,easily available biomass product,is widely applied in sulfate radical-based advanced oxidation processes(SR-AOPs)for emerging pollutants remediation.Herein,a state-of-art revie...In recent years,biochar(BC)as a low-cost,easily available biomass product,is widely applied in sulfate radical-based advanced oxidation processes(SR-AOPs)for emerging pollutants remediation.Herein,a state-of-art review of iron-based biochar catalysts is currently available in SR-AOPs application.A general summary of the development of biochar and the catalytic properties of biochar is presented.Especially,the synthetic strategies of different types of iron-based biochar catalysts are discussed.Moreover,the theoretical calculation to interpret the interaction between biochar and iron species is discussed to explore the activation mechanisms.And the regeneration methods of biochar-based catalyst are presented.The unresolved challenges of the existent biochar-based SR-AOPs are pointed out,and the outlooks of future research directions are proposed.展开更多
Chlorite(ClO_(2)^(−)or COI)is used to establish the advanced reduction and oxidation process(AROP).The iron/biochar-based particles(iron-based hydrothermal carbon with hinge-like structure,FebHCs,20 mg/L)can be utiliz...Chlorite(ClO_(2)^(−)or COI)is used to establish the advanced reduction and oxidation process(AROP).The iron/biochar-based particles(iron-based hydrothermal carbon with hinge-like structure,FebHCs,20 mg/L)can be utilized to activate COI(2 mmol/L)to present selective oxidation in removing triphenylmethane derivatives(15 min,90%).The protonation(H+at~102μmol/L level)played a huge role(k-2nd=0.136c-H+−0.014(R^(2)-adj=0.986),and rapp=−0.0876/c-H++1.017(R^(2)-adj=0.996))to boost the generation of the active species(e.g.,high-valent iron oxidizing species(HVI=O)and chlorine dioxide(ClO_(2))).The protonation-coupled electron transfer promoted Fe-substances in Feb/HCs activating COI(the calculated kobs ranging from 0.066−0.285 min^(−1)).The form of ClO_(2) mainly attributed to proton-coupled electron transfer(1e/1H+).The HVI=O was generated from the electron transfer within the coordination complex.Moreover,carbon particles in FebHCs serve as the bridge for electron transfer.The above roles contribute to the fracture and formation of coordination-induced bonds between Lx-FeII/III and ClO_(2)^(−)at phase interface to form AROP.The ultrasonic(US)cavitation enhanced the mass transfer of active species in bulk solution,and the HVI=O and ClO_(2) attack unsaturated central carbon atoms of triphenylmethane derivatives to initiate selective removal.Furthermore,the scale-up experiment with continuous flow(k values of approximately 0.2 min^(−1),COD removal efficiency of approximately 80%)and the reactor with COMSOL simulation have also proved the applicability of the system.The study offers a novel AROP and new insights into correspondingly heterogeneous interface activation mechanisms.展开更多
Iron-based metal matrix composites(IMMCs)have attracted significant research attention due to their high specific stiffness and strength,making them potentially suitable for various engineering applications.Microstruc...Iron-based metal matrix composites(IMMCs)have attracted significant research attention due to their high specific stiffness and strength,making them potentially suitable for various engineering applications.Microstructural design,including the selection of reinforcement and matrix phases,the reinforcement volume fraction,and the interface issues are essential factors determining the engineering performance of IMMCs.A variety of fabrication methods have been developed to manufacture IMMCs in recent years.This paper reviews the recent advances and development of IMMCs with particular focus on microstructure design,fabrication methods,and their engineering performance.The microstructure design issues of IMMC are firstly discussed,including the reinforcement and matrix phase selection criteria,interface geometry and characteristics,and the bonding mechanism.The fabrication methods,including liquid state,solid state,and gas-mixing processing are comprehensively reviewed and compared.The engineering performance of IMMCs in terms of elastic modulus,hardness and wear resistance,tensile and fracture behavior is reviewed.Finally,the current challenges of the IMMCs are highlighted,followed by the discussion and outlook of the future research directions of IMMCs.展开更多
Increasing environmental pollution and shortage of conventional fossil fuels have made it urgent to develop renewable and clean energy sources. Electrocatalytic water splitting, with its abundant raw materials, simple...Increasing environmental pollution and shortage of conventional fossil fuels have made it urgent to develop renewable and clean energy sources. Electrocatalytic water splitting, with its abundant raw materials, simple process, and zero carbon emission, is considered one of the most promising processes for producing carbon-neutral hydrogen which has excellent energy conversion efficiency and high gravimetric energy density. Among them, oxygen evolution reaction (OER) electrocatalysts and hydrogen evolution reaction (HER) electrocatalysts are critical to decreasing the intrinsic reaction energy barrier and boosting the hydrogen evolution efficiency. Therefore, it is imperative to develop and design low-cost, highly active, and stable OER and HER electrocatalysts to lower the overpotential and drive the electrocatalytic reactions. Transition metal sulfides, especially iron-based sulfides, have attracted extensive exploration by researchers as a result of its high abundance in the Earth's crust and near-metallic conductivity. Consequently, in this review, we systematically and comprehensively summarize the progress in the application of iron-based sulfides and their composites as OER and HER electrocatalysts in electrocatalysis. Detailed descriptions and illustrations of the special relationships among their composition, structure, and electrocatalytic performance are presented. Finally, this review points out the challenges and future prospects of iron-based sulfides in practical applications for designing and fabricating more promising iron-based sulfide OER and HER electrocatalysts. We believe that iron-based sulfide materials will have a wide range of application prospects as OER and HER electrocatalysts in the future.展开更多
Capturing and utilizing CO_(2)from the production process is the key to solving the excessive CO_(2)emission problem. CO_(2)hydrogenation with green hydrogen to produce olefins is an effective and promising way to uti...Capturing and utilizing CO_(2)from the production process is the key to solving the excessive CO_(2)emission problem. CO_(2)hydrogenation with green hydrogen to produce olefins is an effective and promising way to utilize CO_(2)and produce valuable chemicals. The olefins can be produced by CO_(2)hydrogenation through two routes, i.e., CO_(2)-FTS (carbon dioxide Fischer- Tropsch synthesis) and MeOH (methanol-mediated), among which CO_(2)-FTS has significant advantages over MeOH in practical applications due to its relatively high CO_(2)conversion and low energy consumption potentials. However, the CO_(2)-FTS faces challenges of difficult CO_(2)activation and low olefins selectivity. Iron-based catalysts are promising for CO_(2)-FTS due to their dual functionality of catalyzing RWGS and CO-FTS reactions. This review summarizes the recent progress on iron-based catalysts for CO_(2)hydrogenation via the FTS route and analyzes the catalyst optimization from the perspectives of additives, active sites, and reaction mechanisms. Furthermore, we also outline principles and challenges for rational design of high-performance CO_(2)-FTS catalysts.展开更多
Hydrogen sulfide(H_(2)S) not only presents significant environmental concerns but also induces severe corrosion in industrial equipment,even at low concentrations.Among various technologies,the selective oxidation of ...Hydrogen sulfide(H_(2)S) not only presents significant environmental concerns but also induces severe corrosion in industrial equipment,even at low concentrations.Among various technologies,the selective oxidation of hydrogen sulfide(SOH_(2)S) to elemental sulfur(S) has emerged as a sustainable and environmentally friendly solution.Due to its unique properties,iron oxide has been extensively investigated as a catalyst for SOH_(2)S;however,rapid deactivation has remained a significant drawback.The causes of iron oxide-based catalysts deactivation mechanisms in SOH_(2)S,including sulfur or sulfate deposition,the transformation of iron species,sintering and excessive oxygen vacancy formation,and active site loss,are thoroughly examined in this review.By focusing on the deactivation mechanisms,this review aims to provide valuable insights into enhancing the stability and efficiency of iron-based catalysts for SOH_(2)S.展开更多
Anode materials are an essential part of lithium-ion batteries(LIBs),which determine the performance and safety of LIBs.Currently,graphite,as the anode material of commercial LIBs,is limited by its low theoretical cap...Anode materials are an essential part of lithium-ion batteries(LIBs),which determine the performance and safety of LIBs.Currently,graphite,as the anode material of commercial LIBs,is limited by its low theoretical capacity of 372 mA·h·g^(−1),thus hindering further development toward high-capacity and large-scale applications.Alkaline earth metal iron-based oxides are considered a promising candidate to replace graphite because of their low preparation cost,good thermal stability,superior stability,and high electrochemical performance.Nonetheless,many issues and challenges remain to be addressed.Herein,we systematically summarize the research progress of alkaline earth metal iron-based oxides as LIB anodes.Meanwhile,the material and structural properties,synthesis methods,electrochemical reaction mechanisms,and improvement strategies are introduced.Finally,existing challenges and future research directions are discussed to accelerate their practical application in commercial LIBs.展开更多
Heterogeneous iron-based catalysts have drawn increasing attention in the advanced oxidation of persulfates due to their abundance in nature,the lack of secondary pollution to the environment,and their low cost over t...Heterogeneous iron-based catalysts have drawn increasing attention in the advanced oxidation of persulfates due to their abundance in nature,the lack of secondary pollution to the environment,and their low cost over the last a few years.In this paper,the latest progress in the research on the activation of persulfate by heterogeneous iron-based catalysts is reviewed from two aspects,in terms of synthesized catalysts(Fe0,Fe_(2)O_(3),Fe_(3)O_(4),FeOOH)and natural iron ore catalysts(pyrite,magnetite,hematite,siderite,goethite,ferrohydrite,ilmenite and lepidocrocite)focusing on efforts made to improve the performance of catalysts.The advantages and disadvantages of the synthesized catalysts and natural iron ore were summarized.Particular interests were paid to the activation mechanisms in the catalyst/PS/pollutant system for removal of organic pollutants.Future research challenges in the context of field application were also discussed.展开更多
Long-term mulching has improved crop yields and farmland productivity in semiarid areas,but it has also increased greenhouse gas(GHG)emissions and depleted soil fertility.Biochar application has emerged as a promising...Long-term mulching has improved crop yields and farmland productivity in semiarid areas,but it has also increased greenhouse gas(GHG)emissions and depleted soil fertility.Biochar application has emerged as a promising solution for addressing these issues.In this study,we investigated the effects of four biochar application rates(no biochar(N)=0 t ha^(-1),low(L)=3 t ha^(-1),medium(M)=6 t ha^(-1),and high(H)=9 t ha^(-1))under film mulching and no mulching conditions over three growing seasons.We assessed the impacts on GHG emissions,soil organic carbon sequestration(SOCS),and maize yield to evaluate the productivity and sustainability of farmland ecosystems.Our results demonstrated that mulching increased maize yield(18.68-41.80%),total fixed C in straw(23.64%),grain(28.87%),and root(46.31%)biomass,and GHG emissions(CO_(2),10.78%;N_(2)O,3.41%),while reducing SOCS(6.57%)and GHG intensity(GHGI;13.61%).Under mulching,biochar application significantly increased maize yield(10.20%),total fixed C in straw(17.97%),grain(17.69%)and root(16.75%)biomass,and SOCS(4.78%).Moreover,it reduced the GHG emissions(CO_(2),3.09%;N_(2)O,6.36%)and GHGI(12.28%).These effects correlated with the biochar addition rate,with the optimal rate being 9.0 t ha^(-1).In conclusion,biochar application reduces CO_(2) and N_(2)O emissions,enhances CH_(4) absorption,and improves maize yield under film mulching.It also improves the soil carbon fixation capacity while mitigating the warming potential,making it a promising sustainable management method for mulched farmland in semiarid areas.展开更多
Arsenic(As)pollution in soils is a pervasive environmental issue.Biochar immobilization offers a promising solution for addressing soil As contamination.The efficiency of biochar in immobilizing As in soils primarily ...Arsenic(As)pollution in soils is a pervasive environmental issue.Biochar immobilization offers a promising solution for addressing soil As contamination.The efficiency of biochar in immobilizing As in soils primarily hinges on the characteristics of both the soil and the biochar.However,the influence of a specific property on As immobilization varies among different studies,and the development and application of arsenic passivation materials based on biochar often rely on empirical knowledge.To enhance immobilization efficiency and reduce labor and time costs,a machine learning(ML)model was employed to predict As immobilization efficiency before biochar application.In this study,we collected a dataset comprising 182 data points on As immobilization efficiency from 17 publications to construct three ML models.The results demonstrated that the random forest(RF)model outperformed gradient boost regression tree and support vector regression models in predictive performance.Relative importance analysis and partial dependence plots based on the RF model were conducted to identify the most crucial factors influencing As immobilization.These findings highlighted the significant roles of biochar application time and biochar pH in As immobilization efficiency in soils.Furthermore,the study revealed that Fe-modified biochar exhibited a substantial improvement in As immobilization.These insights can facilitate targeted biochar property design and optimization of biochar application conditions to enhance As immobilization efficiency.展开更多
Current research primarily focuses on emerging organic pollutants,with limited attention to emerging inorganic pollutants (EIPs).However,due to advances in detection technology and the escalating environmental and hea...Current research primarily focuses on emerging organic pollutants,with limited attention to emerging inorganic pollutants (EIPs).However,due to advances in detection technology and the escalating environmental and health challenges posed by pollution,there is a growing interest in treating waters contaminated with EIPs.This paper explores biochar characteristics and modification methods,encompassing physical,chemical,and biological approaches for adsorbing EIPs.It offers a comprehensive review of research advancements in employing biochar for EIPs remediation in water,outlines the adsorption mechanisms of EIPs by biochar,and presents an environmental and economic analysis.It can be concluded that using biochar for the adsorption of EIPs in wastewater exhibits promising potential.Nonetheless,it is noteworthy that certain EIPs like Au(III),Rh(III),Ir(III),Ru(III),Os(III),Sc(III),and Y(III),have not been extensively investigated regarding their adsorption onto biochar.This comprehensive review will catalyze further inquiry into the biochar-based adsorption of EIPs,addressing current research deficiencies and advancing the practical implementation of biochar as a potent substrate for EIP removal from wastewater streams.展开更多
Aims:Reed(Phragmites australis)is a plant species with a seasonal reproductive cycle;it has a very high biomass in U Minh Thuong National Park,in Vietnam.This study aims to evaluate fresh and dry biomass of the reed a...Aims:Reed(Phragmites australis)is a plant species with a seasonal reproductive cycle;it has a very high biomass in U Minh Thuong National Park,in Vietnam.This study aims to evaluate fresh and dry biomass of the reed and the production of biochar from the plants.The biochar is then used as a bio-organic fertilizer for watermelon cultivation in agriculture.Methods:To achieve these objectives the following experiments were conducted(1)investtigating the fresh and dry biomass of reeds producing biochar using local methods;(2)adsorption with pig urine and chemical fertilizers(nitrogen,phosphorus and potash)to examine the uptake of chemical components into the water environment;(3)mixing biochar with inorganic mineral fertilizers and peat to creat inorganic fertilizer–biochar formulas,followed by an analysis of the chemical compositions of the mixtures;(4)using various biochar-based fertilizers to grow watermelon with local varieties.Results:The results show that reeds produce very high for biomass biochar fertilizer production.Reed biochar can adsorb components of pig urine,such as ammonium,nitrate,nitrogen and phosphorus along with inorganic substances such as nitrogen,phosphorus and potash.Therefore this study proposes the use of this biochar for watermelon cultivation and environment treatment in polluted regions.Conclusions:Biomass and biochar of reed are very high.The biochar can adsorb nitrogen,phosphorus and potash fertilizers.Additionally,biochar can be mixed with peat and inorganic mineral fertilizers for to watermelon cultivation in Mekong Delta.Implications of the research:Forest fires in U Minh Thuong National Park,caused by reed vegetation,occur annually and result in damage to property and human livelihoods.This research not only exploits renewable raw materials but also helps control the risk of forest fires.Originality/Valeu:This study aims to provide methods for controlling forest fires by producing biochar of from reed(Phragmites australis)U Minh Thuong National Park Vietnam.This species thrives and produces a large biomass during the rainy season,supllying dry material that contributes to the intensity of forest fires in the dry season in Vietnam.展开更多
Dibromoethane is a widespread,persistent organic pollutant.Biochars are known mediators of reductive dehalogenation by layered Fe^(Ⅱ)-Fe^(Ⅲ)hydroxides(green rust),which can reduce 1,2-dibromoethane to innocuous brom...Dibromoethane is a widespread,persistent organic pollutant.Biochars are known mediators of reductive dehalogenation by layered Fe^(Ⅱ)-Fe^(Ⅲ)hydroxides(green rust),which can reduce 1,2-dibromoethane to innocuous bromide and ethylene.However,the critical characteristics that determine mediator functionality are lesser known.Fifteen biochar substrates were pyrolyzed at 600℃and 800℃,characterized by elemental analysis,X-ray photo spectrometry C and N surface speciation,X-ray powder diffraction,specific surface area analysis,and tested for mediation of reductive debromination of 1,2-dibromoethane by a green rust reductant under anoxic conditions.A statistical analysis was performed to determine the biochar properties,critical for debromination kinetics and total debromination extent.It was shown that selected plant based biochars can mediate debromination of 1,2-dibromoethane,that the highest first order rate constant was 0.082/hr,and the highest debromination extent was 27%in reactivity experiments with 0.1μmol(20μmol/L)1,2-dibromoethane,≈22 mmol/L Fe^(Ⅱ)GR,and 0.12 g/L soybean meal biochar(7 days).Contents of Ni,Zn,N,and P,and the relative contribution of quinone surface functional groups were significantly(p<0.05)positively correlated with 1,2-dibromoethane debromination,while adsorption,specific surface area,and the relative contribution of pyridinic N oxide surface groups were significantly negatively correlated with debromination.展开更多
In this study,two wheat-derived cadmium(Cd)-immobilizing endophytic Pseudomonas paralactis M14 and Priestia megaterium R27 were evaluated for their effects on wheat tissue Cd uptake under hydroponic conditions.Then,th...In this study,two wheat-derived cadmium(Cd)-immobilizing endophytic Pseudomonas paralactis M14 and Priestia megaterium R27 were evaluated for their effects on wheat tissue Cd uptake under hydroponic conditions.Then,the impacts of the biochar(BC),M14+R27(MR),and BC+MR treatments on wheat Cd uptake and the mechanisms involved were investigated at the jointing,heading,and mature stages of wheat plants under field-plot conditions.A hydroponic experiment showed that the MR treatment significantly decreased the above-ground tissue Cd content compared with theM14 or R27 treatment.The BC+MRtreatment reduced the grain Cd content by 51.5%-67.7%and Cd translocation factor at the mature stage of wheat plants and increased the organic matter-bound Cd content by 31%-75%in the rhizosphere soils compared with the BC or MR treatment.Compared with the BC or MR treatment,the relative abundances of the biomarkers associated with Gemmatimonas,Altererythrobacter,Gammaproteobacteria,Xanthomonadaceae,Phenylobacterium,and Nocardioides in the BC+MR-treated rhizosphere microbiome decreased and negatively correlated with the organic matter-bound Cd contents.In the BC+MR-treated root interior microbiome,the relative abundance of the biomarker belonging to Exiguobacterium increased and negatively correlated with the Cd translocation factor,while the relative abundance of the biomarker belonging to Pseudonocardiaceae decreased and positively correlated with the Cd translocation factor.Our findings suggested that the BC+MR treatment reduced Cd availability and Cd transfer through affecting the abundances of these specific biomarkers in the rhizosphere soil and root interior microbiomes,leading to decreased wheat grain Cd uptake in the contaminated soil.展开更多
Superconducting transition temperature(Tc),as a crucial parameter,exploring its relationship with various macroscopic and microscopic factors helps to understand the mechanism of high-temperature superconductivity fro...Superconducting transition temperature(Tc),as a crucial parameter,exploring its relationship with various macroscopic and microscopic factors helps to understand the mechanism of high-temperature superconductivity from multiple perspectives,aiding in a multidimensional comprehension of high-temperature superconductivity mechanisms.Drawing inspiration from the block-layer structure models of cuprate superconductors,we computationally investigated the interlayer interaction energies in the 12442-type iron-based superconducting materials AkCa_(2)Fe_(4)As_(4)F_(2)(Ak=K,Rb,Cs)systems based on the block-layer model and explored their relationship with Tc.We observed that an increase in interlayer combinative energy leads to a decrease in Tc,while conversely,a decrease in interlayer combination energy results in an increase in Tc.Further,we found that the contribution of the Fe 3d band structure,especially the 3dz2 orbital,to charge transfer is significant.展开更多
The technology for green and macro-conversion of solid waste biomass to prepare high-quality activated carbon demands urgent development.This study proposes a technique for synthesizing carbon adsorbents using trace K...The technology for green and macro-conversion of solid waste biomass to prepare high-quality activated carbon demands urgent development.This study proposes a technique for synthesizing carbon adsorbents using trace KOH-catalyzed CO_(2) activation.Comprehensive investigations were conducted on three aspects:physicochemical structure evolution of biochar,mechanistic understanding of trace KOH-facilitated CO_(2) activation processes,and application characteristics for CO_(2) adsorption.Results demonstrate that biochar activated by trace KOH(<10%)and CO_(2) achieves comparable specific surface area(1244.09 m^(2)/g)to that obtained with 100%KOH activation(1425.10 m^(2)/g).The pore structure characteristics(specific surface area and pore volume)are governed by CO and CH4 generated through K-salt catalyzed reactions between CO_(2) and biochar.The optimal CO_(2) adsorption capacities of KBC adsorbent reached 4.70 mmol/g(0℃)and 7.25 mmol/g(25℃),representing the maximum values among comparable carbon adsorbents.The 5%KBC-CO_(2) sample exhibited CO_(2) adsorption capacities of 3.19 and 5.01 mmol/g under respective conditions,attaining current average performance levels.Notably,CO_(2)/N_(2) selectivity(85∶15,volume ratio)reached 64.71 at 0.02 bar with robust cycling stability.Molecular dynamics simulations revealed that oxygen-containing functional groups accelerate CO_(2) adsorption kinetics and enhance micropore storage capacity.This technical route offers simplicity,environmental compatibility,and scalability,providing critical references for large-scale preparation of high-quality carbon materials.展开更多
Biomass-derived heteroatom self-doped cathode catalysts has attracted considerable interest for electrochemical advanced oxidation processes(EAOPs)due to its high performance and sustainable synthesis.Herein,we illust...Biomass-derived heteroatom self-doped cathode catalysts has attracted considerable interest for electrochemical advanced oxidation processes(EAOPs)due to its high performance and sustainable synthesis.Herein,we illustrated the morphological fates of waste leaf-derived graphitic carbon(WLGC)produced from waste ginkgo leaves via pyrolysis temperature regulation and used as bifunctional cathode catalyst for simultaneous H_(2)O_(2) electrochemical generation and organic pollutant degradation,discovering S/N-self-doping shown to facilitate a synergistic effect on reactive oxygen species(ROS)generation.Under the optimum temperature of 800℃,the WLGC exhibited a H_(2)O_(2) selectivity of 94.2%and tetracycline removal of 99.3%within 60 min.Density functional theory calculations and in-situ Fourier transformed infrared spectroscopy verified that graphitic N was the critical site for H_(2)O_(2) generation.While pyridinic N and thiophene S were the main active sites responsible for OH generation,N vacancies were the active sites to produce ^(1)O_(2) from O_(2).The performance of the novel cathode for tetracycline degradation remains well under a wide pH range(3–11),maintaining excellent stability in 10 cycles.It is also industrially applicable,achieving satisfactory performance treating in real water matrices.This system facilitates both radical and non-radical degradation,offering valuable advances in the preparation of cost-effective and sustainable electrocatalysts and hold strong potentials in metal-free EAOPs for organic pollutant degradation.展开更多
Harnessing the redox potential of biochar to activate airborne O_(2)for contaminant removal is challenging.In this study,ferrihydrite(Fh)modified the boron(B),nitrogen(N)co-doped biochars(BCs)composites(Fh/B(n)NC)were...Harnessing the redox potential of biochar to activate airborne O_(2)for contaminant removal is challenging.In this study,ferrihydrite(Fh)modified the boron(B),nitrogen(N)co-doped biochars(BCs)composites(Fh/B(n)NC)were developed for enhancing the degradation of a model pollutant,tetracycline(TC),merely by airborne O_(2).Fh/B(3)NC showed excellent O_(2)activation activity for efficient TC degradation with a apparent TC degradation rate of 5.54,6.88,and 22.15 times that of B(3)NC,Fh,and raw BCs,respectively,where 1O_(2)and H_(2)O_(2)were identified as the dominant ROS for TC degradation.The B incorporation into the carbon lattice of Fh/B(3)NC promoted the generation of electron donors,sp2 C and the reductive B species,hence boosting Fe(III)reduction and 1O_(2)generation.O_(2)adsorption was enhanced due to the positively charged adsorption sites(C-B+and N-C+).And 1O_(2)was generated via Fe(II)catalyzed low-efficient successive one-electron transfer(O_(2)→O_(2)·−→1O_(2),H_(2)O_(2)),as well as biochar catalyzed high-efficient two-electron transfer(O_(2)→H_(2)O_(2)→1O_(2))that does not involve.O_(2)−as the intermediate.Moreover,Fh/B,N co-doped biochar showed a wide pH range,remarkable anti-interference capabilities,and effective detoxification.These findings shed new light on the development of environmentally benign BCs materials capable of degradading organic pollutants.展开更多
Humic acid(HA),as a represent of natural organic matter widely existing in water body,dose harm to water quality and human health;however,it was commonly treated as an environmental background substance while not targ...Humic acid(HA),as a represent of natural organic matter widely existing in water body,dose harm to water quality and human health;however,it was commonly treated as an environmental background substance while not targeted contaminant in advanced oxidation processes(AOPs).Herein,we investigated the removal of HA in the alkali-activated biochar(KBC)/peroxymonosulfate(PMS)system.The modification of the original biochar(BC)resulted in an increased adsorption capacity and catalytic activity due to the introduction of more micropores,mesopores,and oxygen-containing functional groups,particularly carbonyl groups.Mechanistic insights indicated that HA is primarily chemically adsorbed on the KBC surface,while singlet oxygen(^(1)O_(2))produced by the PMS decomposition served as the major reactive species for the degradation of HA.An underlying synergistic adsorption and oxidation mechanism involving a local high concentration reaction region around the KBC interface was then proposed.This work not only provides a cost-effective solution for the elimination of HA but also advances our understanding of the nonradical oxidation at the biochar interface.展开更多
Dissolved organic matter(DOM)is ubiquitous in the environment and plays an important role in global ecosystems.However,our understanding of the evolution and molecular diversity of DOM from different biomass materials...Dissolved organic matter(DOM)is ubiquitous in the environment and plays an important role in global ecosystems.However,our understanding of the evolution and molecular diversity of DOM from different biomass materials and biochar is not enough.Herein,we investigated the changes in DOM from seven biomass and biochar samples over a bio-incubation of 28 days,and explored their contents,and optical,chemical,and molecular characteristics.The results indicated that dissolved organic carbon(DOC)from different sources all exhibited a gradually decreasing trends during the incubation,while the absorbance and aromaticity gradually increased.Biomass DOM was characterized by higher DOC concentrations and a higher degradation rate,whereas biochar DOM had high aromaticity and little variability.Parallel factor analysis results showed that the protein-like fluorescent groups were as only detected in biomass DOM,while the dominant humic-like components were identified in biochar DOM.Additionally,the molecular composition of DOM from different sources was different,and biomass DOM contained more carbohydrate-like and saturated compounds.More sulfur-containing compounds were detected in Ceratophyllum demersum(CD)DOM,which may indicate that the leaching of CD litter was an important source of sulfur-containing species in aquatic environments.Furthermore,biochar DOM had greater aromaticity and a higher degree of oxidation than the corresponding biomass DOM.This study provided a detailed understanding of the molecular diversity of DOM by considering its various sources,and the results are helpful for further understanding their chemical properties and structures.展开更多
基金supported by the National Natural Science Foundation of China(No.51778230).
文摘In recent years,biochar(BC)as a low-cost,easily available biomass product,is widely applied in sulfate radical-based advanced oxidation processes(SR-AOPs)for emerging pollutants remediation.Herein,a state-of-art review of iron-based biochar catalysts is currently available in SR-AOPs application.A general summary of the development of biochar and the catalytic properties of biochar is presented.Especially,the synthetic strategies of different types of iron-based biochar catalysts are discussed.Moreover,the theoretical calculation to interpret the interaction between biochar and iron species is discussed to explore the activation mechanisms.And the regeneration methods of biochar-based catalyst are presented.The unresolved challenges of the existent biochar-based SR-AOPs are pointed out,and the outlooks of future research directions are proposed.
基金supported by the Natural Science foundation of the Jiangsu Higher Education Institutions(No.24KJB610019)the Scientific Research Foundation of Yancheng Teachers University(No.204060047)the Horizontal Topic Research“Developing the environmental remediation technology by acoustic catalysis”(No.203060199).
文摘Chlorite(ClO_(2)^(−)or COI)is used to establish the advanced reduction and oxidation process(AROP).The iron/biochar-based particles(iron-based hydrothermal carbon with hinge-like structure,FebHCs,20 mg/L)can be utilized to activate COI(2 mmol/L)to present selective oxidation in removing triphenylmethane derivatives(15 min,90%).The protonation(H+at~102μmol/L level)played a huge role(k-2nd=0.136c-H+−0.014(R^(2)-adj=0.986),and rapp=−0.0876/c-H++1.017(R^(2)-adj=0.996))to boost the generation of the active species(e.g.,high-valent iron oxidizing species(HVI=O)and chlorine dioxide(ClO_(2))).The protonation-coupled electron transfer promoted Fe-substances in Feb/HCs activating COI(the calculated kobs ranging from 0.066−0.285 min^(−1)).The form of ClO_(2) mainly attributed to proton-coupled electron transfer(1e/1H+).The HVI=O was generated from the electron transfer within the coordination complex.Moreover,carbon particles in FebHCs serve as the bridge for electron transfer.The above roles contribute to the fracture and formation of coordination-induced bonds between Lx-FeII/III and ClO_(2)^(−)at phase interface to form AROP.The ultrasonic(US)cavitation enhanced the mass transfer of active species in bulk solution,and the HVI=O and ClO_(2) attack unsaturated central carbon atoms of triphenylmethane derivatives to initiate selective removal.Furthermore,the scale-up experiment with continuous flow(k values of approximately 0.2 min^(−1),COD removal efficiency of approximately 80%)and the reactor with COMSOL simulation have also proved the applicability of the system.The study offers a novel AROP and new insights into correspondingly heterogeneous interface activation mechanisms.
基金funding support from the National Natural Science Foundation of China(No.52101046)Shuangjie Chu appreciates the funding support from the National Key Research and Development Program of China(No.2022YFB3705600).
文摘Iron-based metal matrix composites(IMMCs)have attracted significant research attention due to their high specific stiffness and strength,making them potentially suitable for various engineering applications.Microstructural design,including the selection of reinforcement and matrix phases,the reinforcement volume fraction,and the interface issues are essential factors determining the engineering performance of IMMCs.A variety of fabrication methods have been developed to manufacture IMMCs in recent years.This paper reviews the recent advances and development of IMMCs with particular focus on microstructure design,fabrication methods,and their engineering performance.The microstructure design issues of IMMC are firstly discussed,including the reinforcement and matrix phase selection criteria,interface geometry and characteristics,and the bonding mechanism.The fabrication methods,including liquid state,solid state,and gas-mixing processing are comprehensively reviewed and compared.The engineering performance of IMMCs in terms of elastic modulus,hardness and wear resistance,tensile and fracture behavior is reviewed.Finally,the current challenges of the IMMCs are highlighted,followed by the discussion and outlook of the future research directions of IMMCs.
基金the National Natural Science Foundation of China(No.22275052)the Natural Science Foundation of Hubei Province(No.2019CFB569)。
文摘Increasing environmental pollution and shortage of conventional fossil fuels have made it urgent to develop renewable and clean energy sources. Electrocatalytic water splitting, with its abundant raw materials, simple process, and zero carbon emission, is considered one of the most promising processes for producing carbon-neutral hydrogen which has excellent energy conversion efficiency and high gravimetric energy density. Among them, oxygen evolution reaction (OER) electrocatalysts and hydrogen evolution reaction (HER) electrocatalysts are critical to decreasing the intrinsic reaction energy barrier and boosting the hydrogen evolution efficiency. Therefore, it is imperative to develop and design low-cost, highly active, and stable OER and HER electrocatalysts to lower the overpotential and drive the electrocatalytic reactions. Transition metal sulfides, especially iron-based sulfides, have attracted extensive exploration by researchers as a result of its high abundance in the Earth's crust and near-metallic conductivity. Consequently, in this review, we systematically and comprehensively summarize the progress in the application of iron-based sulfides and their composites as OER and HER electrocatalysts in electrocatalysis. Detailed descriptions and illustrations of the special relationships among their composition, structure, and electrocatalytic performance are presented. Finally, this review points out the challenges and future prospects of iron-based sulfides in practical applications for designing and fabricating more promising iron-based sulfide OER and HER electrocatalysts. We believe that iron-based sulfide materials will have a wide range of application prospects as OER and HER electrocatalysts in the future.
基金the National Natural Science Foundation of China-Outstanding Youth Foundation (No. 22322814)the National Natural Science Foundation of China (No. 22108144)the Natural Science Foundation of Shandong-Outstanding Youth Foundation (No. ZR2023YQ017)。
文摘Capturing and utilizing CO_(2)from the production process is the key to solving the excessive CO_(2)emission problem. CO_(2)hydrogenation with green hydrogen to produce olefins is an effective and promising way to utilize CO_(2)and produce valuable chemicals. The olefins can be produced by CO_(2)hydrogenation through two routes, i.e., CO_(2)-FTS (carbon dioxide Fischer- Tropsch synthesis) and MeOH (methanol-mediated), among which CO_(2)-FTS has significant advantages over MeOH in practical applications due to its relatively high CO_(2)conversion and low energy consumption potentials. However, the CO_(2)-FTS faces challenges of difficult CO_(2)activation and low olefins selectivity. Iron-based catalysts are promising for CO_(2)-FTS due to their dual functionality of catalyzing RWGS and CO-FTS reactions. This review summarizes the recent progress on iron-based catalysts for CO_(2)hydrogenation via the FTS route and analyzes the catalyst optimization from the perspectives of additives, active sites, and reaction mechanisms. Furthermore, we also outline principles and challenges for rational design of high-performance CO_(2)-FTS catalysts.
基金supported by Thailand Science Research and Innovation Fund Chulalongkorn University,Thailand(IND66210014)。
文摘Hydrogen sulfide(H_(2)S) not only presents significant environmental concerns but also induces severe corrosion in industrial equipment,even at low concentrations.Among various technologies,the selective oxidation of hydrogen sulfide(SOH_(2)S) to elemental sulfur(S) has emerged as a sustainable and environmentally friendly solution.Due to its unique properties,iron oxide has been extensively investigated as a catalyst for SOH_(2)S;however,rapid deactivation has remained a significant drawback.The causes of iron oxide-based catalysts deactivation mechanisms in SOH_(2)S,including sulfur or sulfate deposition,the transformation of iron species,sintering and excessive oxygen vacancy formation,and active site loss,are thoroughly examined in this review.By focusing on the deactivation mechanisms,this review aims to provide valuable insights into enhancing the stability and efficiency of iron-based catalysts for SOH_(2)S.
基金The authors acknowledge the support of the Shenyang University of Technology(QNPY202209-4)the National Natural Science Foundation of China(21571132)+1 种基金Jiangsu University Advanced Talent Fund(5501710002)the Education Department of Liaoning Province(JYTQN2023285).
文摘Anode materials are an essential part of lithium-ion batteries(LIBs),which determine the performance and safety of LIBs.Currently,graphite,as the anode material of commercial LIBs,is limited by its low theoretical capacity of 372 mA·h·g^(−1),thus hindering further development toward high-capacity and large-scale applications.Alkaline earth metal iron-based oxides are considered a promising candidate to replace graphite because of their low preparation cost,good thermal stability,superior stability,and high electrochemical performance.Nonetheless,many issues and challenges remain to be addressed.Herein,we systematically summarize the research progress of alkaline earth metal iron-based oxides as LIB anodes.Meanwhile,the material and structural properties,synthesis methods,electrochemical reaction mechanisms,and improvement strategies are introduced.Finally,existing challenges and future research directions are discussed to accelerate their practical application in commercial LIBs.
基金supported by the National Natural Science Foundation of China(No.52170071)the Natural Science Foundation of Guangdong Province(No.2022A1515011909)the Natural Science Foundation of Xiamen(No.3502Z20227187).
文摘Heterogeneous iron-based catalysts have drawn increasing attention in the advanced oxidation of persulfates due to their abundance in nature,the lack of secondary pollution to the environment,and their low cost over the last a few years.In this paper,the latest progress in the research on the activation of persulfate by heterogeneous iron-based catalysts is reviewed from two aspects,in terms of synthesized catalysts(Fe0,Fe_(2)O_(3),Fe_(3)O_(4),FeOOH)and natural iron ore catalysts(pyrite,magnetite,hematite,siderite,goethite,ferrohydrite,ilmenite and lepidocrocite)focusing on efforts made to improve the performance of catalysts.The advantages and disadvantages of the synthesized catalysts and natural iron ore were summarized.Particular interests were paid to the activation mechanisms in the catalyst/PS/pollutant system for removal of organic pollutants.Future research challenges in the context of field application were also discussed.
基金supported by the National Key Research and Development Program of China(2021YFE0101300 and 2021YFD1901102)the project supported by the Natural Science Basic Research Plan in Shaanxi Province,China(2023-JC-YB-185)the Ningxia Key Research and Development Program,China(2023BCF01018)。
文摘Long-term mulching has improved crop yields and farmland productivity in semiarid areas,but it has also increased greenhouse gas(GHG)emissions and depleted soil fertility.Biochar application has emerged as a promising solution for addressing these issues.In this study,we investigated the effects of four biochar application rates(no biochar(N)=0 t ha^(-1),low(L)=3 t ha^(-1),medium(M)=6 t ha^(-1),and high(H)=9 t ha^(-1))under film mulching and no mulching conditions over three growing seasons.We assessed the impacts on GHG emissions,soil organic carbon sequestration(SOCS),and maize yield to evaluate the productivity and sustainability of farmland ecosystems.Our results demonstrated that mulching increased maize yield(18.68-41.80%),total fixed C in straw(23.64%),grain(28.87%),and root(46.31%)biomass,and GHG emissions(CO_(2),10.78%;N_(2)O,3.41%),while reducing SOCS(6.57%)and GHG intensity(GHGI;13.61%).Under mulching,biochar application significantly increased maize yield(10.20%),total fixed C in straw(17.97%),grain(17.69%)and root(16.75%)biomass,and SOCS(4.78%).Moreover,it reduced the GHG emissions(CO_(2),3.09%;N_(2)O,6.36%)and GHGI(12.28%).These effects correlated with the biochar addition rate,with the optimal rate being 9.0 t ha^(-1).In conclusion,biochar application reduces CO_(2) and N_(2)O emissions,enhances CH_(4) absorption,and improves maize yield under film mulching.It also improves the soil carbon fixation capacity while mitigating the warming potential,making it a promising sustainable management method for mulched farmland in semiarid areas.
基金supported by the National Key Research and Development Program of China(No.2020YFC1808701).
文摘Arsenic(As)pollution in soils is a pervasive environmental issue.Biochar immobilization offers a promising solution for addressing soil As contamination.The efficiency of biochar in immobilizing As in soils primarily hinges on the characteristics of both the soil and the biochar.However,the influence of a specific property on As immobilization varies among different studies,and the development and application of arsenic passivation materials based on biochar often rely on empirical knowledge.To enhance immobilization efficiency and reduce labor and time costs,a machine learning(ML)model was employed to predict As immobilization efficiency before biochar application.In this study,we collected a dataset comprising 182 data points on As immobilization efficiency from 17 publications to construct three ML models.The results demonstrated that the random forest(RF)model outperformed gradient boost regression tree and support vector regression models in predictive performance.Relative importance analysis and partial dependence plots based on the RF model were conducted to identify the most crucial factors influencing As immobilization.These findings highlighted the significant roles of biochar application time and biochar pH in As immobilization efficiency in soils.Furthermore,the study revealed that Fe-modified biochar exhibited a substantial improvement in As immobilization.These insights can facilitate targeted biochar property design and optimization of biochar application conditions to enhance As immobilization efficiency.
基金support from the earmarked fund for XJARS(No.XJARS-06)the Bingtuan Science and Technology Program(Nos.2021DB019,2022CB001-01)+1 种基金the National Natural Science Foundation of China(No.42275014)the Guangdong Foundation for Program of Science and Technology Research,China(No.2023B1212060044)。
文摘Current research primarily focuses on emerging organic pollutants,with limited attention to emerging inorganic pollutants (EIPs).However,due to advances in detection technology and the escalating environmental and health challenges posed by pollution,there is a growing interest in treating waters contaminated with EIPs.This paper explores biochar characteristics and modification methods,encompassing physical,chemical,and biological approaches for adsorbing EIPs.It offers a comprehensive review of research advancements in employing biochar for EIPs remediation in water,outlines the adsorption mechanisms of EIPs by biochar,and presents an environmental and economic analysis.It can be concluded that using biochar for the adsorption of EIPs in wastewater exhibits promising potential.Nonetheless,it is noteworthy that certain EIPs like Au(III),Rh(III),Ir(III),Ru(III),Os(III),Sc(III),and Y(III),have not been extensively investigated regarding their adsorption onto biochar.This comprehensive review will catalyze further inquiry into the biochar-based adsorption of EIPs,addressing current research deficiencies and advancing the practical implementation of biochar as a potent substrate for EIP removal from wastewater streams.
文摘Aims:Reed(Phragmites australis)is a plant species with a seasonal reproductive cycle;it has a very high biomass in U Minh Thuong National Park,in Vietnam.This study aims to evaluate fresh and dry biomass of the reed and the production of biochar from the plants.The biochar is then used as a bio-organic fertilizer for watermelon cultivation in agriculture.Methods:To achieve these objectives the following experiments were conducted(1)investtigating the fresh and dry biomass of reeds producing biochar using local methods;(2)adsorption with pig urine and chemical fertilizers(nitrogen,phosphorus and potash)to examine the uptake of chemical components into the water environment;(3)mixing biochar with inorganic mineral fertilizers and peat to creat inorganic fertilizer–biochar formulas,followed by an analysis of the chemical compositions of the mixtures;(4)using various biochar-based fertilizers to grow watermelon with local varieties.Results:The results show that reeds produce very high for biomass biochar fertilizer production.Reed biochar can adsorb components of pig urine,such as ammonium,nitrate,nitrogen and phosphorus along with inorganic substances such as nitrogen,phosphorus and potash.Therefore this study proposes the use of this biochar for watermelon cultivation and environment treatment in polluted regions.Conclusions:Biomass and biochar of reed are very high.The biochar can adsorb nitrogen,phosphorus and potash fertilizers.Additionally,biochar can be mixed with peat and inorganic mineral fertilizers for to watermelon cultivation in Mekong Delta.Implications of the research:Forest fires in U Minh Thuong National Park,caused by reed vegetation,occur annually and result in damage to property and human livelihoods.This research not only exploits renewable raw materials but also helps control the risk of forest fires.Originality/Valeu:This study aims to provide methods for controlling forest fires by producing biochar of from reed(Phragmites australis)U Minh Thuong National Park Vietnam.This species thrives and produces a large biomass during the rainy season,supllying dry material that contributes to the intensity of forest fires in the dry season in Vietnam.
文摘Dibromoethane is a widespread,persistent organic pollutant.Biochars are known mediators of reductive dehalogenation by layered Fe^(Ⅱ)-Fe^(Ⅲ)hydroxides(green rust),which can reduce 1,2-dibromoethane to innocuous bromide and ethylene.However,the critical characteristics that determine mediator functionality are lesser known.Fifteen biochar substrates were pyrolyzed at 600℃and 800℃,characterized by elemental analysis,X-ray photo spectrometry C and N surface speciation,X-ray powder diffraction,specific surface area analysis,and tested for mediation of reductive debromination of 1,2-dibromoethane by a green rust reductant under anoxic conditions.A statistical analysis was performed to determine the biochar properties,critical for debromination kinetics and total debromination extent.It was shown that selected plant based biochars can mediate debromination of 1,2-dibromoethane,that the highest first order rate constant was 0.082/hr,and the highest debromination extent was 27%in reactivity experiments with 0.1μmol(20μmol/L)1,2-dibromoethane,≈22 mmol/L Fe^(Ⅱ)GR,and 0.12 g/L soybean meal biochar(7 days).Contents of Ni,Zn,N,and P,and the relative contribution of quinone surface functional groups were significantly(p<0.05)positively correlated with 1,2-dibromoethane debromination,while adsorption,specific surface area,and the relative contribution of pyridinic N oxide surface groups were significantly negatively correlated with debromination.
基金supported by the National Natural Science Foundation of China(No.41977199).
文摘In this study,two wheat-derived cadmium(Cd)-immobilizing endophytic Pseudomonas paralactis M14 and Priestia megaterium R27 were evaluated for their effects on wheat tissue Cd uptake under hydroponic conditions.Then,the impacts of the biochar(BC),M14+R27(MR),and BC+MR treatments on wheat Cd uptake and the mechanisms involved were investigated at the jointing,heading,and mature stages of wheat plants under field-plot conditions.A hydroponic experiment showed that the MR treatment significantly decreased the above-ground tissue Cd content compared with theM14 or R27 treatment.The BC+MRtreatment reduced the grain Cd content by 51.5%-67.7%and Cd translocation factor at the mature stage of wheat plants and increased the organic matter-bound Cd content by 31%-75%in the rhizosphere soils compared with the BC or MR treatment.Compared with the BC or MR treatment,the relative abundances of the biomarkers associated with Gemmatimonas,Altererythrobacter,Gammaproteobacteria,Xanthomonadaceae,Phenylobacterium,and Nocardioides in the BC+MR-treated rhizosphere microbiome decreased and negatively correlated with the organic matter-bound Cd contents.In the BC+MR-treated root interior microbiome,the relative abundance of the biomarker belonging to Exiguobacterium increased and negatively correlated with the Cd translocation factor,while the relative abundance of the biomarker belonging to Pseudonocardiaceae decreased and positively correlated with the Cd translocation factor.Our findings suggested that the BC+MR treatment reduced Cd availability and Cd transfer through affecting the abundances of these specific biomarkers in the rhizosphere soil and root interior microbiomes,leading to decreased wheat grain Cd uptake in the contaminated soil.
文摘Superconducting transition temperature(Tc),as a crucial parameter,exploring its relationship with various macroscopic and microscopic factors helps to understand the mechanism of high-temperature superconductivity from multiple perspectives,aiding in a multidimensional comprehension of high-temperature superconductivity mechanisms.Drawing inspiration from the block-layer structure models of cuprate superconductors,we computationally investigated the interlayer interaction energies in the 12442-type iron-based superconducting materials AkCa_(2)Fe_(4)As_(4)F_(2)(Ak=K,Rb,Cs)systems based on the block-layer model and explored their relationship with Tc.We observed that an increase in interlayer combinative energy leads to a decrease in Tc,while conversely,a decrease in interlayer combination energy results in an increase in Tc.Further,we found that the contribution of the Fe 3d band structure,especially the 3dz2 orbital,to charge transfer is significant.
基金supported by the National Natural Science Foundation of China(52376103,542B2081).
文摘The technology for green and macro-conversion of solid waste biomass to prepare high-quality activated carbon demands urgent development.This study proposes a technique for synthesizing carbon adsorbents using trace KOH-catalyzed CO_(2) activation.Comprehensive investigations were conducted on three aspects:physicochemical structure evolution of biochar,mechanistic understanding of trace KOH-facilitated CO_(2) activation processes,and application characteristics for CO_(2) adsorption.Results demonstrate that biochar activated by trace KOH(<10%)and CO_(2) achieves comparable specific surface area(1244.09 m^(2)/g)to that obtained with 100%KOH activation(1425.10 m^(2)/g).The pore structure characteristics(specific surface area and pore volume)are governed by CO and CH4 generated through K-salt catalyzed reactions between CO_(2) and biochar.The optimal CO_(2) adsorption capacities of KBC adsorbent reached 4.70 mmol/g(0℃)and 7.25 mmol/g(25℃),representing the maximum values among comparable carbon adsorbents.The 5%KBC-CO_(2) sample exhibited CO_(2) adsorption capacities of 3.19 and 5.01 mmol/g under respective conditions,attaining current average performance levels.Notably,CO_(2)/N_(2) selectivity(85∶15,volume ratio)reached 64.71 at 0.02 bar with robust cycling stability.Molecular dynamics simulations revealed that oxygen-containing functional groups accelerate CO_(2) adsorption kinetics and enhance micropore storage capacity.This technical route offers simplicity,environmental compatibility,and scalability,providing critical references for large-scale preparation of high-quality carbon materials.
基金financially supported by National Key R&D Program International Cooperation Project(2023YFE0108100)Natural Science Foundation of China(No.52170085)+2 种基金Key Project of Natural Science Foundation of Tianjin(No.21JCZDJC00320)Tianjin Post-graduate Students Research and Innovation Project(2021YJSB013)Fundamental Research Funds for the Central Universities,Nankai University.
文摘Biomass-derived heteroatom self-doped cathode catalysts has attracted considerable interest for electrochemical advanced oxidation processes(EAOPs)due to its high performance and sustainable synthesis.Herein,we illustrated the morphological fates of waste leaf-derived graphitic carbon(WLGC)produced from waste ginkgo leaves via pyrolysis temperature regulation and used as bifunctional cathode catalyst for simultaneous H_(2)O_(2) electrochemical generation and organic pollutant degradation,discovering S/N-self-doping shown to facilitate a synergistic effect on reactive oxygen species(ROS)generation.Under the optimum temperature of 800℃,the WLGC exhibited a H_(2)O_(2) selectivity of 94.2%and tetracycline removal of 99.3%within 60 min.Density functional theory calculations and in-situ Fourier transformed infrared spectroscopy verified that graphitic N was the critical site for H_(2)O_(2) generation.While pyridinic N and thiophene S were the main active sites responsible for OH generation,N vacancies were the active sites to produce ^(1)O_(2) from O_(2).The performance of the novel cathode for tetracycline degradation remains well under a wide pH range(3–11),maintaining excellent stability in 10 cycles.It is also industrially applicable,achieving satisfactory performance treating in real water matrices.This system facilitates both radical and non-radical degradation,offering valuable advances in the preparation of cost-effective and sustainable electrocatalysts and hold strong potentials in metal-free EAOPs for organic pollutant degradation.
基金supported by the National Natural Science Foundation of China(No.U21A20293).
文摘Harnessing the redox potential of biochar to activate airborne O_(2)for contaminant removal is challenging.In this study,ferrihydrite(Fh)modified the boron(B),nitrogen(N)co-doped biochars(BCs)composites(Fh/B(n)NC)were developed for enhancing the degradation of a model pollutant,tetracycline(TC),merely by airborne O_(2).Fh/B(3)NC showed excellent O_(2)activation activity for efficient TC degradation with a apparent TC degradation rate of 5.54,6.88,and 22.15 times that of B(3)NC,Fh,and raw BCs,respectively,where 1O_(2)and H_(2)O_(2)were identified as the dominant ROS for TC degradation.The B incorporation into the carbon lattice of Fh/B(3)NC promoted the generation of electron donors,sp2 C and the reductive B species,hence boosting Fe(III)reduction and 1O_(2)generation.O_(2)adsorption was enhanced due to the positively charged adsorption sites(C-B+and N-C+).And 1O_(2)was generated via Fe(II)catalyzed low-efficient successive one-electron transfer(O_(2)→O_(2)·−→1O_(2),H_(2)O_(2)),as well as biochar catalyzed high-efficient two-electron transfer(O_(2)→H_(2)O_(2)→1O_(2))that does not involve.O_(2)−as the intermediate.Moreover,Fh/B,N co-doped biochar showed a wide pH range,remarkable anti-interference capabilities,and effective detoxification.These findings shed new light on the development of environmentally benign BCs materials capable of degradading organic pollutants.
基金supported by the National Natural Science Foundation of China(No.52200049)the China Postdoctoral Science Foundation(No.2022TQ0089)the Heilongjiang Province Postdoctoral Science Foundation(No.LBHZ22181).
文摘Humic acid(HA),as a represent of natural organic matter widely existing in water body,dose harm to water quality and human health;however,it was commonly treated as an environmental background substance while not targeted contaminant in advanced oxidation processes(AOPs).Herein,we investigated the removal of HA in the alkali-activated biochar(KBC)/peroxymonosulfate(PMS)system.The modification of the original biochar(BC)resulted in an increased adsorption capacity and catalytic activity due to the introduction of more micropores,mesopores,and oxygen-containing functional groups,particularly carbonyl groups.Mechanistic insights indicated that HA is primarily chemically adsorbed on the KBC surface,while singlet oxygen(^(1)O_(2))produced by the PMS decomposition served as the major reactive species for the degradation of HA.An underlying synergistic adsorption and oxidation mechanism involving a local high concentration reaction region around the KBC interface was then proposed.This work not only provides a cost-effective solution for the elimination of HA but also advances our understanding of the nonradical oxidation at the biochar interface.
基金supported by the National Natural Science Foundation of China(No.42192514)Guangdong Major Project of Basic and Applied Basic Research(No.2023B0303000007)and Guangdong Foundation for Program of Science and Technology Research(No.2023B1212060049)。
文摘Dissolved organic matter(DOM)is ubiquitous in the environment and plays an important role in global ecosystems.However,our understanding of the evolution and molecular diversity of DOM from different biomass materials and biochar is not enough.Herein,we investigated the changes in DOM from seven biomass and biochar samples over a bio-incubation of 28 days,and explored their contents,and optical,chemical,and molecular characteristics.The results indicated that dissolved organic carbon(DOC)from different sources all exhibited a gradually decreasing trends during the incubation,while the absorbance and aromaticity gradually increased.Biomass DOM was characterized by higher DOC concentrations and a higher degradation rate,whereas biochar DOM had high aromaticity and little variability.Parallel factor analysis results showed that the protein-like fluorescent groups were as only detected in biomass DOM,while the dominant humic-like components were identified in biochar DOM.Additionally,the molecular composition of DOM from different sources was different,and biomass DOM contained more carbohydrate-like and saturated compounds.More sulfur-containing compounds were detected in Ceratophyllum demersum(CD)DOM,which may indicate that the leaching of CD litter was an important source of sulfur-containing species in aquatic environments.Furthermore,biochar DOM had greater aromaticity and a higher degree of oxidation than the corresponding biomass DOM.This study provided a detailed understanding of the molecular diversity of DOM by considering its various sources,and the results are helpful for further understanding their chemical properties and structures.
