A mesocosm-based study was conducted to assess the effect of glucose and hydrogen peroxide on periphyton communities. These chemicals have been found to be effective at controlling cyanobacteria blooms in the water co...A mesocosm-based study was conducted to assess the effect of glucose and hydrogen peroxide on periphyton communities. These chemicals have been found to be effective at controlling cyanobacteria blooms in the water column but their impact on attached communities is unknown. The experimental design included a total of 4 treatments: control (no chemicals;3 replicates);hydrogen peroxide (3 replicates);glucose alone (3 different concentrations [no replicates]);and additive glucose (3 replicates). After 34 days, mean values of chlorophyll a were lower in all experimental treatments compared to the control;mean AFDM values were lower in all treatments except the unreplicated high glucose alone treatment. In contrast, mean autotrophic index values (AFDM/chlorophyll a) were greater in all treatments compared to the control, indicating heterotrophs were more resistant to the chemical treatments than autotrophs. Periphyton community biodiversity was much lower in the additive glucose and moderate glucose alone treatments than the hydrogen peroxide and control treatments. The relative abundance of the bacteria Asticcacaulis and Sphingorhabdus responded positively to the glucose treatments, whereas relative abundance of Nevskia and Caenimonas declined in both the hydrogen peroxide and glucose treatments. In terms of relative abundance, no cyanobacteria taxa were detected among the top 20 taxa. We conclude that the autotrophic component of periphyton communities is especially vulnerable to hydrogen peroxide and glucose treatments, and that any management strategy employing these chemicals should be aware of this potential impact.展开更多
Pyrrhotite oxidation poses a big threat to water environment duo to its high potential for generating pollutants.Hydrogen peroxide,commonly found in natural water at micromolar concentrations,possesses much more aggre...Pyrrhotite oxidation poses a big threat to water environment duo to its high potential for generating pollutants.Hydrogen peroxide,commonly found in natural water at micromolar concentrations,possesses much more aggressive oxidation ability than oxygen and can complicate the pyrrhotite oxidation process.Here,the effects of micromolar H_(2)O_(2) on the biotic and abiotic oxidation of pyrrhotite were examined at pH 1.93 and 6.45,respectively.Pyrrhotite oxidation was much more severe in acidic solutions compared to near neutral solutions.Jarosite with a high Fe/S molar ratio was widely detected in the precipitate collected in acidic solutions,and the introduction of external H_(2)O_(2) influenced the crystallinity of jarosite.A layer of iron-deficient iron-sulfur oxide formed on the surface of pyrrhotite prevents its continuous oxidation,and the presence of Acidithiobacillus ferrooxidans enhanced this situation by promoting the release of Fe from the pyrrhotite.Additionally,the presence of external micromolar H_(2)O_(2) also determined the elemental state on pyrrhotite surface,as it found that the contribution of Fe^(3+)and S(S^(4+)and S^(6+))species on pyrrhotite surface increased with the increase of H_(2)O_(2) concentration in the solutions,especially in the presence of Acidithiobacillus ferrooxidans.展开更多
Enhancing rubber-bitumen compatibility is crucial to improve pavement performance and durability.To investigate the compatibility improvement between H2O2-activated waste crumb rubber(AWCR)and bitumen,coarse and fine ...Enhancing rubber-bitumen compatibility is crucial to improve pavement performance and durability.To investigate the compatibility improvement between H2O2-activated waste crumb rubber(AWCR)and bitumen,coarse and fine waste crumb rubber(WCR)were treated and analyzed through multi-scale characterization and molecular simulation.Microstructure and chemical changes of WCR and AWCR were analyzed with scanning electron microscope(SEM),contact angle tests and Fourier transform infrared spectroscopy(FTIR).Compatibility was also indirectly evaluated through modified boiling tests and storage stability tests.Besides,molecular dynamics was used to explore the interaction between WCR/AWCR and bitumen.SEM,contact angle,and FTIR results showed bond breakage of C=C and C–C and increased polar groups like–OH and–COOH in AWCR,resulting in a rougher texture and higher surface energy.Compared with WCR,AWCR showed a lower bitumen stripping rate after boiling,and the binder with AWCR also had a lower softening point difference and segregation rate after storage.Molecular dynamics simulations further confirmed that AWCR has a closer solubility parameter and higher binding energy to bitumen than WCR,reflected in a relatively slower diffusion rate.This study provides comprehensive evidence for an eco-friendly method of WCR surface treatment for more efficient recycling of tire rubber in asphalt pavements.展开更多
This letter addresses Pravda's innovative review,which proposes hydrogen pe-roxide as the primary pathogenic factor in ulcerative colitis(UC).Although the author presents intriguing mechanistic insights and report...This letter addresses Pravda's innovative review,which proposes hydrogen pe-roxide as the primary pathogenic factor in ulcerative colitis(UC).Although the author presents intriguing mechanistic insights and reports encouraging clinical outcomes with reducing agents,several methodological and clinical considera-tions require discussion.We examine three key aspects:The selective evidence synthesis approach;the need for rigorous clinical validation of proposed thera-pies;and the integration of this novel hypothesis with established inflammatory bowel disease pathogenesis.Given the complexity of UC,future therapeutic ad-vances may require collaborative approaches that integrate redox-based mecha-nisms into existing evidence-based frameworks rather than replacing current paradigms.展开更多
The photocatalytic hydrogen peroxide(H_(2)O_(2))production by graphitic carbon nitride is a sustainable and environment-benign alternative approach of conventional anthraquinone autoxidation technology,but it is great...The photocatalytic hydrogen peroxide(H_(2)O_(2))production by graphitic carbon nitride is a sustainable and environment-benign alternative approach of conventional anthraquinone autoxidation technology,but it is great challenges to promote two-electron O_(2)reduction and water oxidation.Herein,we present the well-dispersed graphitic carbon nitride quantum dots decorated with cyano groups(Na-CNQD and K-CNQD)by thermal polymerization of melamine in the presence of metal fluoride.The quantum confinement and edge effect have endowed the photocatalysts with rich active sites,wide light absorption range and the inhibited charge recombination.The cyano moieties function as O_(2)reduction centers to accept the photogenerated electrons and facilitate their rapid transfer to O_(2)molecules.This process enables the selective two-electron reduction of O_(2),leading to the production of H_(2)O_(2).Concurrently,the valence band holes on the heptazine moiety oxidize water into H_(2)O_(2).These synergistic effects promote photocatalytic H_(2)O_(2)production from O_(2)and H_(2)O without the need for additional photosensitizers,organic scavengers and co-catalysts.In contrast,pristine carbon nitride nanosheets remain inactive under the same conditions.This study offers new strategies for rational design of carbon-based materials for solar-to-chemical energy conversion.展开更多
Mesenchymal stem cells(MSCs)possess unique properties such as immunomodu-lation,paracrine actions,multilineage differentiation,and self-renewal.Therefore,MSC-based cell therapy is an innovative approach to treating va...Mesenchymal stem cells(MSCs)possess unique properties such as immunomodu-lation,paracrine actions,multilineage differentiation,and self-renewal.Therefore,MSC-based cell therapy is an innovative approach to treating various degenera-tive illnesses,including cardiovascular diseases.However,several challenges,including low transplant survival rates,low migration to the ischemic myocar-dium,and poor tissue retention,restrict the application of MSCs in clinical settings.These undesirable cell therapy outcomes mainly originated due to the overproduction of reactive oxygen species(ROS)in the injured heart.MSCs'stress-coping capacity can be enhanced by preconditioning them under conditions similar to the microenvironment of wounded tissues.Hydrogen peroxide(H_(2)O_(2))is a ROS that has been shown to activate protective cellular mechanisms such as survival,proliferation,migration,paracrine effects,and differentiation at suble-thal doses.These processes are induced via phosphatidylinositol 3-kinase/protein kinase B,p38 mitogen-activated protein kinases,c-Jun N-terminal kinase,Janus kinase/signal transducer and activator of the transcription,Notch1,and Wnt sig-naling pathways.H_(2)O_(2) preconditioning could lead to many clinical benefits,including ischemic injury reduction,enhanced survival of cellular transplants,and tissue regeneration.In this review,we present an overview of stem cell preconditioning methods and the biological functions activated by H_(2)O_(2) precondi-tioning.Furthermore,this review explores the molecular mechanisms underlying the protective cellular functions stimulated under H_(2)O_(2) preconditioning.展开更多
Cobalt pentlandite(Co9S8)is a promising non-precious catalyst due to its superior oxygen reduction reaction activity and excellent stability.However,its oxygen reduction reaction catalytic activity has traditionally b...Cobalt pentlandite(Co9S8)is a promising non-precious catalyst due to its superior oxygen reduction reaction activity and excellent stability.However,its oxygen reduction reaction catalytic activity has traditionally been limited to the four-electron pathway because of strong*OOH intermediate adsorption.In this study,we synthesized electron-deficient Co9S8 nanocrystals with an increased number of Co^(3+)states compared to conventional Co9S8.This was achieved by incorporating a high density of surface ligands in small-sized Co9S8nanocrystals,which enabled the transition of the electrochemical reduction pathway from four-electron oxygen reduction reaction to two-electron oxygen reduction reaction by decreasing*OOH adsorption strength.As a result,the Co^(3+)-enriched Co9S8 nanocrystals exhibited a high onset potential of 0.64 V(vs RHE)for two-electron oxygen reduction reaction,achieving H_(2)O_(2) selectivity of 70-80%over the potential range from 0.05 to 0.6 V.Additionally,these nanocrystals demonstrated a stable H_(2)O_(2) electrosynthesis at a rate of459.12 mmol g^(-1) h^(-1) with a H_(2)O_(2) Faradaic efficiency over 90%under alkaline conditions.This study provides insights into nanoscale catalyst design for modulating electrochemical reactions.展开更多
As a versatile and environmentally benign oxidant,hydrogen peroxide(H_(2)O_(2))is highly desired in sanitation,disinfection,environmental remediation,and the chemical industry.Compared with the conventional anthraquin...As a versatile and environmentally benign oxidant,hydrogen peroxide(H_(2)O_(2))is highly desired in sanitation,disinfection,environmental remediation,and the chemical industry.Compared with the conventional anthraquinone process,the electrosynthesis of H_(2)O_(2)through the two-electron oxygen reduction reaction(2e^(−)ORR)is an efficient,competitive,and promising avenue.Electrocatalysts and devices are two core factors in 2e^(−)ORR,but the design principles of catalysts for different pH conditions and the development trends of relevant synthesis devices remain unclear.To this end,this review adopts a multiscale perspective to summarize recent advancements in the design principles,catalytic mechanisms,and application prospects of 2e^(−)ORR catalysts,with a particular focus on the influence of pH conditions,aiming at providing guidance for the selective design of advanced 2e^(−)ORR catalysts for highly-efficient H_(2)O_(2)production.Moreover,in response to diverse on-site application demands,we elaborate on the evolution of H_(2)O_(2)electrosynthesis devices,from rotating ring-disk electrodes and H-type cells to diverse flow-type cells.We elaborate on their characteristics and shortcomings,which can be beneficial for their further upgrades and customized applications.These insights may inspire the rational design of innovative catalysts and devices with high performance and wide serviceability for large-scale implementations.展开更多
Hydrogen peroxide(H_(2)O_(2))is an eco-friendly chemical with widespread industrial applications.However,the commercial anthraquinone process for H_(2)O_(2) production is energy-intensive and environmentally harmful,h...Hydrogen peroxide(H_(2)O_(2))is an eco-friendly chemical with widespread industrial applications.However,the commercial anthraquinone process for H_(2)O_(2) production is energy-intensive and environmentally harmful,highlighting the need for more sustainable alternatives.The electrochemical production of H_(2)O_(2) via the two-electron water oxidation reaction(2e^(−)WOR)presents a promising route but is often hindered by low efficiency and selectivity,due to the competition with the oxygen evolution reaction.In this study,we employed high-throughput computational screening and microkinetic modeling to design a series of efficient 2e^(−)WOR electrocatalysts from a library of 240 single-metal-embedded nitrogen heterocycle aromatic molecules(M-NHAMs).These catalysts,primarily comprising post-transition metals,such as Cu,Ni,Zn,and Pd,exhibit high activity for H_(2)O_(2) conversion with a limiting potential approaching the optimal value of 1.76 V.Additionally,they exhibit excellent selectivity,with Faradaic efficiencies exceeding 80%at overpotentials below 300 mV.Structure-performance analysis reveals that the d-band center and magnetic moment of the metal center correlated strongly with the oxygen adsorption free energy(ΔGO*),suggesting these parameters as key catalytic descriptors for efficient screening and performance optimization.This study contributes to the rational design of highly efficient and selective electrocatalysts for electrochemical production of H_(2)O_(2),offering a sustainable solution for green energy and industrial applications.展开更多
BACKGROUND Fistula-in-ano is an abnormal tunnel formation linking the anal canal with the perineum and perianal skin.Multiple imagining methods are available to evaluate it,among which magnetic resonance imaging(MRI)i...BACKGROUND Fistula-in-ano is an abnormal tunnel formation linking the anal canal with the perineum and perianal skin.Multiple imagining methods are available to evaluate it,among which magnetic resonance imaging(MRI)is the most advanced nonin-vasive preoperative method.However,it is limited in its visualization function.AIM To investigate the use of intraluminal MRI for perianal fistulas via a novel direct MRI fistulography method.METHODS We mixed 3%hydrogen peroxide(HP)with gadolinium for HPMRI fistulogra-phy,retrospectively analyzing 60 cases of complex/recurrent fistula-in-ano using physical examination,trans-perineal ultrasonography(TPUS),low-spatial-reso-lution MRI,and high-resolution direct HPMRI fistulography.We assessed detec-tion rates of fistula tracks,internal openings,their relationship with anal sphinc-ters,and perianal abscesses using statistical analyses,including interobserver agreement(Kappa statistic),and compared results with intraoperative findings.RESULTS Surgical confirmation in 60 cases showed that high-resolution direct HPMRI fis-tulography provided superior detection rates for internal openings(153)and fistula tracks(162)compared to physical exams,TPUS,and low-spatial-resolution MRI(Z>5.7,P<0.05).The effectiveness of physical examination and TPUS was also inferior to that of our method for detecting perianal abscesses(54)(Z=6.773,3.694,P<0.05),whereas that of low-spatial-resolution MRI was not significantly different(Z=1.851,P=0.06).High-resolution direct HPMRI fistulography also achieved the highest interobserver agreement(Kappa:0.89,0.85,and 0.80),while low-spatial-resolution MRI showed moderate agreement(Kappa:0.78,0.74,and 0.69).TPUS and physical examination had lower agreement(Kappa range:0.33-0.63).CONCLUSION High-resolution direct HPMRI fistulography enhances the visualization of recurrent and complex fistula-in-ano,including branched fistulas,allowing for precise planning and improved surgical outcomes.展开更多
Photocatalytic hydrogen peroxide(H_(2)O_(2))production offers a sustainable route to convert water and oxygen into H_(2)O_(2)using solar energy.However,achieving long-term stability in photocatalysts remains a critica...Photocatalytic hydrogen peroxide(H_(2)O_(2))production offers a sustainable route to convert water and oxygen into H_(2)O_(2)using solar energy.However,achieving long-term stability in photocatalysts remains a critical challenge due to mismatched kinetics between oxygen reduction(ORR)and water oxidation(WOR),which leads to hole accumulation and oxidative degradation.Here,we report a redox-mediated strategy to address this bottleneck by designing a hydroquinone-embedded covalent organic framework(Tz-QH-COF)that enables reversible hole buffering and kinetic balance.The hydroquinone(QH)units act as dynamic hole reservoirs,capturing excess holes during ORR and converting to benzoquinone(Q),which is regenerated to QH via WOR,thereby preventing oxidative decomposition.This reversible QH/Q cycle,directly visualized through in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy,ensures unmatched stability,achieving continuous H_(2)O_(2) production for 528 h(22 d)with an accumulated yield of 18.6 mmol L^(–1)—the highest reported duration for organic photocatalysts.Density functional theory calculations reveal that the QH units exhibit a strong oxygen adsorption energy and favorable two-electron ORR/WOR pathways with low energy barriers.The synergy between experimental and theoretical insights elucidates a redox-mediated charge-balance mechanism,advancing the design of robust photocatalysts for solar-driven H_(2)O_(2) synthesis.展开更多
Advanced oxidation processes(AOPs)governed by peroxide activation to produce highly oxidative active species have been extensively explored for environmental remediation.Nevertheless,the low diffusion rates,inadequate...Advanced oxidation processes(AOPs)governed by peroxide activation to produce highly oxidative active species have been extensively explored for environmental remediation.Nevertheless,the low diffusion rates,inadequate interactions of the reactants,and limited active site exposure hinder treatment efficiency.Porous carbocatalysts with high specific surface area,tunable pore size,and programmable active sites demonstrate outstanding performance in activating diverse types of peroxides to generate active species for treatment of aqueous organic pollutants.The pore-rich structures enhance reaction kinetics for peroxide activation by facilitating diffusion of the reactants and their interactions.Additionally,the structural flexibility of porous structures favors the accommodation of highly dispersed metal species and allows for precise tuning of the microenvironment around the active sites,which further enhances the catalytic activity.This review critically summarizes the recent research progress in the applications of engineered porous carbocatalysts for peroxide activation and outlines the prevailing pore construction methods in carbocatalysts.Moreover,engineering strategies to regulate the mass transfer efficiency and fine-tune the microenvironment around the active sites are systematically addressed to enhance their catalytic peroxide activation performances.Challenges and future research opportunities pertaining to the design,optimization,mechanistic investigation,and practical application of porous carbocatalysts in peroxide activation are also proposed.展开更多
BACKGROUND Current disinfection methods for gastrointestinal endoscopes consume a significant amount of water resources and produce a large volume of waste.AIM To achieve the objectives of efficiency,speed,and cost-ef...BACKGROUND Current disinfection methods for gastrointestinal endoscopes consume a significant amount of water resources and produce a large volume of waste.AIM To achieve the objectives of efficiency,speed,and cost-effectiveness,this study utilized vaporized hydrogen peroxide(VHP)generated from sodium percarbonate granules to conduct an anhydrous disinfection test on gastrointestinal endoscopes.METHODS The experimental device rapidly converts sodium percarbonate granules into VHP,and performs disinfection experiments on gastrointestinal endoscope models,disposable endoscopes,and various types of reusable gastrointestinal endoscopes.Variables such as the intraluminal flow rate(FR),relative humidity(RH),exposure dosage,and organic burden are used to explore the factors influencing the disinfection of long and narrow lumens with VHP.RESULTS The device generates a certain concentration of VHP that can achieve high-level disinfection of endoscope models within 30 minutes.RH,exposure dosage,and organic burden significantly affect the disinfection efficacy of VHP,whereas the intraluminal FR does not significantly impact disinfection efficacy.All ten artificially contaminated disposable endoscopes achieved satisfactory disinfection results.Furthermore,when this device was used to treat various types of reusable endoscopes,the disinfection and sterilization effects were not significantly different from those of automatic endoscope disinfection machines(using peracetic acid disinfectant solution)(P>0.05),and the economic cost of disinfectant required per endoscope was lower(1.5 China Yuan),with a shorter disinfection time(30 minutes).CONCLUSION The methods and results of this study provide a basis for further research on the use of VHP for the disinfection of gastrointestinal endoscopes,as well as for the development of anhydrous disinfection technology for gastrointestinal endoscopes.展开更多
In this editorial,a commentary on the article by Chang et al has been provided,the course of treatment of anorectal fistulas,especially complex and recurring ones,require accurate diagnostic procedures for determining...In this editorial,a commentary on the article by Chang et al has been provided,the course of treatment of anorectal fistulas,especially complex and recurring ones,require accurate diagnostic procedures for determining ideal surgical procedures.Conventional ways of imaging sometimes fall short,offering insufficient insights in aggravated instances.In this editorial,a novel application of hydrogen peroxide-enhanced magnetic resonance imaging(HP-MRI)that promises significant improvements in the imaging of anorectal fistula.Study is based on a retrospective investigation of 60 patients,contrasts the new HP-MRI with conventional diagnostic techniques such as physical examination,trans-perineal ultrasonography and poor spatial resolution MRI.The findings demonstrate HP-MRI's incredible diagnostic performance,with sensitivity and specificity rates of 96.08%and 90.91%,respectively,and unparalleled interobserver agreement(Kappa values ranging from 0.80 to 0.89).It has been a significant advancement for assessment of anorectal fistulas providing a better roadmap for surgical planning,lowering recurrence rates as well as reduced personal and financial burden on patients by reducing the need for repeated treatment and extended hospital stays.The remaining funds can be utilized for treatment of other medical need.Ultimately HP-MRI provides us a healthier&more efficient society by improvising patients well-being&optimized healthcare infrastructure.展开更多
Photocatalytic production of hydrogen peroxide(H_(2)O_(2))presents a promising strategy for environmental remediation and energy production.However,achieving clean and efficient H_(2)O_(2) production under ambient con...Photocatalytic production of hydrogen peroxide(H_(2)O_(2))presents a promising strategy for environmental remediation and energy production.However,achieving clean and efficient H_(2)O_(2) production under ambient conditions without organic sacrificial agents remains challenging.Enhancing the low crystallinity of covalent organic frameworks(COFs)can promote the separation and transmission of photo-generated carriers,thereby boosting their photocatalytic performance.Herein,we introduce a novel synthetic approach by substituting traditional acetic acid catalysts with organic base catalysts to enhance the crystallinity of β-ketoenamine-linked COF,TpBD-COF.Compared to TpBD-COF-A synthesized using acetic acid catalysts,TpBD-COF-B,synthesized with organic base catalysts,exhibited advancements including increased absorption intensity in the visible spectrum,reduced photoluminescence intensity,enhanced photo-generated carrier separation performance,and a 2.1-fold increase in photocatalytic H_(2)O_(2) production.Under visible light irradiation,TpBDCOF-B achieved a photocatalytic H_(2)O_(2) production rate of 533μmol/h/g using only air and water,without the need for organic sacrificial agents.Furthermore,TpBD-COF-B also exhibited good performance in long-term catalytic production experiments,tests with actual water bodies,and cyclic usage experiments.This study offers a strategy for enhancing the crystallinity of COFs to improve their photocatalytic activity,with promising applications in clean energy production and environmental remediation.展开更多
Selective electrocatalysis of two-electron oxygen reduction reaction(2e^(-)ORR)has been recognized as a sustainable and on-site process for hydrogen peroxide(H_(2)O_(2))production.Great progress has been achieved for ...Selective electrocatalysis of two-electron oxygen reduction reaction(2e^(-)ORR)has been recognized as a sustainable and on-site process for hydrogen peroxide(H_(2)O_(2))production.Great progress has been achieved for 2e^(-)ORR in alkaline media.However,it is challenged by insufficient activity and selectiv-ity of the catalysts in acidic electrolytes.Herein,we report sulfur-poisoned PtNi/C catalysts(PtNiSx/C)that could regulate ORR from the 4e^(-)to 2e^(-)pathway.The identified PtNiS0.6/C offers high activity in terms of onset potential of∼0.69 V(vs.RHE)and∼80%selectivity.The mass activity is also compara-ble and outperforms representative Pt-based precious and transition-metal-based catalysts.In addition,it is interestingly found that the Faradaic efficiency further increased to 95%during the long-term elec-trolysis test due to Ni atom surface migration.The electrochemical production of the H_(2)O_(2)system was applied to the electro-Fenton process,which has realized the effective degradation of organic pollutants.This work offers a strategy by sulfur poisoning PtNi/C catalyst to realize Pt-based 2e^(-)ORR active catalysts to electrolysis of H_(2)O_(2)in acidic media.展开更多
Degradation of nitrobenzene(NB)via Fenton-like reaction is considered as an efficient approach for contaminated groundwater remediation.However,the poor stability of H2O2limits the application of traditional Fenton re...Degradation of nitrobenzene(NB)via Fenton-like reaction is considered as an efficient approach for contaminated groundwater remediation.However,the poor stability of H2O2limits the application of traditional Fenton reactions in soil and groundwater due to the transportation risks of H_(2)O_(2).In this study,we synthesized a controlled release nano calcium peroxide(n CP)by coating it with polydopamine(PDA)as a solid H2O2to construct a Fe(Ⅱ)/PDA@n CP Fenton-like system for contaminants degradation.The phenolquinone transformations of catechol groups on the PDA surface facilitated the Fe(Ⅱ)/Fe(Ⅲ)cycle,resulting in enhanced generation of hydroxyl radicals(HO·)and effective long-term degradation of NB.Moreover,the PDA shell modulated the n CP decomposition rate and inhibited sharp p H fluctuations,and the NB removal efficiency was achieved up to 96.8%at p H ranging from 3.0 to 9.0.This study demonstrated the promising application potential of PDA@n CP as a solid-controlled release H2O2source in Fenton-like system for groundwater contamination remediation.展开更多
Hydrogen peroxide(H_(2)O_(2))is a crucial,eco-friendly oxidizing agent with a wide range of industrial,environmental,and biomedical applications.Traditional production methods,such as the anthraquinone process,face si...Hydrogen peroxide(H_(2)O_(2))is a crucial,eco-friendly oxidizing agent with a wide range of industrial,environmental,and biomedical applications.Traditional production methods,such as the anthraquinone process,face significant challenges in terms of energy consumption and environmental impact.As a sustainable alternative,photocatalytic H_(2)O_(2) production,driven by solar energy,has emerged as a promising approach.This review discusses the key advancements in photocatalytic H_(2)O_(2) synthesis,focusing on overcoming challenges such as charge recombination,selectivity for the two-electron oxygen reduction reaction(2e^(-)ORR),and catalyst stability.Recent innovations in photocatalyst design,including high-entropy materials,single-atom catalysts,and covalent organic frameworks(COFs),have significantly enhanced efficiency and stability.Furthermore,novel strategies for optimizing charge separation,light harvesting,and mass transfer are explored.The integration of artificial intelligence and bioinspired systems holds potential for accelerating progress in this field.This review provides a comprehensive overview of current challenges and cutting-edge solutions,offering valuable insights for the development of scalable,decentralized H_(2)O_(2) production systems that contribute to a more sustainable future.展开更多
Propylene oxide(PO),with its reactive three-membered epoxide functional group,exhibits remarkable functional versatility and serves as a crucial bridge connecting the gaps between fossil energy utilization and chemica...Propylene oxide(PO),with its reactive three-membered epoxide functional group,exhibits remarkable functional versatility and serves as a crucial bridge connecting the gaps between fossil energy utilization and chemical intermediate generation for new material innovation [1].For instance,PO's downstream derivatives,such as polyether polyols,carbonic esters,and polyurethanes,are widely utilized in wind power generation,battery electrolytes,solar cells,and CO_(2)-based degradable polymers,contributing to sustainable decarbonization in industry [2].展开更多
Photocatalytic technology has attracted much attention in the fields of clean energy and environmental governance.However,how to design and develop highly efficient photocatalytic materials remains an urgent scientifi...Photocatalytic technology has attracted much attention in the fields of clean energy and environmental governance.However,how to design and develop highly efficient photocatalytic materials remains an urgent scientific problem to be solved.This study focuses on enhancing photocatalytic activity through microstructure modification.Among them,ToRed-4 showed the most prominent performance.Under the illumination condition of 420 nm,its value was 13506 lmol g^(-1) h^(-1),which was approximately 18 times that of CN550(bulk g-C_(3)N_(4))(719 lmol g^(-1) h^(-1)).By using DFT calculations,the photocatalytic performance was deeply analyzed,revealing the significant advantages of the ToRed series in key performance indicators and the underlying synergy mechanisms,including the reduction of the HOMO-LUMO energy gap,the efficient separation of electron holes,the expansion of the electronic transition range,the transformation of the electrostatic potential distribution,the increase in dipole moment,and the optimization of the Coulomb attractive energy.The research results of this study provide a key basis for opening up new avenues for the design and development of highly efficient photocatalytic materials and are expected to play an important role in related fields.展开更多
文摘A mesocosm-based study was conducted to assess the effect of glucose and hydrogen peroxide on periphyton communities. These chemicals have been found to be effective at controlling cyanobacteria blooms in the water column but their impact on attached communities is unknown. The experimental design included a total of 4 treatments: control (no chemicals;3 replicates);hydrogen peroxide (3 replicates);glucose alone (3 different concentrations [no replicates]);and additive glucose (3 replicates). After 34 days, mean values of chlorophyll a were lower in all experimental treatments compared to the control;mean AFDM values were lower in all treatments except the unreplicated high glucose alone treatment. In contrast, mean autotrophic index values (AFDM/chlorophyll a) were greater in all treatments compared to the control, indicating heterotrophs were more resistant to the chemical treatments than autotrophs. Periphyton community biodiversity was much lower in the additive glucose and moderate glucose alone treatments than the hydrogen peroxide and control treatments. The relative abundance of the bacteria Asticcacaulis and Sphingorhabdus responded positively to the glucose treatments, whereas relative abundance of Nevskia and Caenimonas declined in both the hydrogen peroxide and glucose treatments. In terms of relative abundance, no cyanobacteria taxa were detected among the top 20 taxa. We conclude that the autotrophic component of periphyton communities is especially vulnerable to hydrogen peroxide and glucose treatments, and that any management strategy employing these chemicals should be aware of this potential impact.
基金supported by the National Key Research and Development Program of China(No.2022YFC3203301)the Natural Science Foundation of China(No.41406098).
文摘Pyrrhotite oxidation poses a big threat to water environment duo to its high potential for generating pollutants.Hydrogen peroxide,commonly found in natural water at micromolar concentrations,possesses much more aggressive oxidation ability than oxygen and can complicate the pyrrhotite oxidation process.Here,the effects of micromolar H_(2)O_(2) on the biotic and abiotic oxidation of pyrrhotite were examined at pH 1.93 and 6.45,respectively.Pyrrhotite oxidation was much more severe in acidic solutions compared to near neutral solutions.Jarosite with a high Fe/S molar ratio was widely detected in the precipitate collected in acidic solutions,and the introduction of external H_(2)O_(2) influenced the crystallinity of jarosite.A layer of iron-deficient iron-sulfur oxide formed on the surface of pyrrhotite prevents its continuous oxidation,and the presence of Acidithiobacillus ferrooxidans enhanced this situation by promoting the release of Fe from the pyrrhotite.Additionally,the presence of external micromolar H_(2)O_(2) also determined the elemental state on pyrrhotite surface,as it found that the contribution of Fe^(3+)and S(S^(4+)and S^(6+))species on pyrrhotite surface increased with the increase of H_(2)O_(2) concentration in the solutions,especially in the presence of Acidithiobacillus ferrooxidans.
基金supported by the research project“Green-health-safety Nexus for New Urban Spaces-GreeNexUS”(HORIZON MSCA-2021 DN,Marie Sklodowska-Curie Actions)Grant Agreement No.101073437:research grant under the title"Impact Absorbing Pavements with Improved Accessibility Features(DC9-IAP)".
文摘Enhancing rubber-bitumen compatibility is crucial to improve pavement performance and durability.To investigate the compatibility improvement between H2O2-activated waste crumb rubber(AWCR)and bitumen,coarse and fine waste crumb rubber(WCR)were treated and analyzed through multi-scale characterization and molecular simulation.Microstructure and chemical changes of WCR and AWCR were analyzed with scanning electron microscope(SEM),contact angle tests and Fourier transform infrared spectroscopy(FTIR).Compatibility was also indirectly evaluated through modified boiling tests and storage stability tests.Besides,molecular dynamics was used to explore the interaction between WCR/AWCR and bitumen.SEM,contact angle,and FTIR results showed bond breakage of C=C and C–C and increased polar groups like–OH and–COOH in AWCR,resulting in a rougher texture and higher surface energy.Compared with WCR,AWCR showed a lower bitumen stripping rate after boiling,and the binder with AWCR also had a lower softening point difference and segregation rate after storage.Molecular dynamics simulations further confirmed that AWCR has a closer solubility parameter and higher binding energy to bitumen than WCR,reflected in a relatively slower diffusion rate.This study provides comprehensive evidence for an eco-friendly method of WCR surface treatment for more efficient recycling of tire rubber in asphalt pavements.
文摘This letter addresses Pravda's innovative review,which proposes hydrogen pe-roxide as the primary pathogenic factor in ulcerative colitis(UC).Although the author presents intriguing mechanistic insights and reports encouraging clinical outcomes with reducing agents,several methodological and clinical considera-tions require discussion.We examine three key aspects:The selective evidence synthesis approach;the need for rigorous clinical validation of proposed thera-pies;and the integration of this novel hypothesis with established inflammatory bowel disease pathogenesis.Given the complexity of UC,future therapeutic ad-vances may require collaborative approaches that integrate redox-based mecha-nisms into existing evidence-based frameworks rather than replacing current paradigms.
基金supported by the National Natural Science Foundation of China(22361024 and 22471055)Natural Science Foundation of Jiangxi Province(20232ACB203001)+1 种基金Natural Science Foundation of Hebei Province(B2024202021,B2022202039)S&T Program of Hebei(236Z4308G)。
文摘The photocatalytic hydrogen peroxide(H_(2)O_(2))production by graphitic carbon nitride is a sustainable and environment-benign alternative approach of conventional anthraquinone autoxidation technology,but it is great challenges to promote two-electron O_(2)reduction and water oxidation.Herein,we present the well-dispersed graphitic carbon nitride quantum dots decorated with cyano groups(Na-CNQD and K-CNQD)by thermal polymerization of melamine in the presence of metal fluoride.The quantum confinement and edge effect have endowed the photocatalysts with rich active sites,wide light absorption range and the inhibited charge recombination.The cyano moieties function as O_(2)reduction centers to accept the photogenerated electrons and facilitate their rapid transfer to O_(2)molecules.This process enables the selective two-electron reduction of O_(2),leading to the production of H_(2)O_(2).Concurrently,the valence band holes on the heptazine moiety oxidize water into H_(2)O_(2).These synergistic effects promote photocatalytic H_(2)O_(2)production from O_(2)and H_(2)O without the need for additional photosensitizers,organic scavengers and co-catalysts.In contrast,pristine carbon nitride nanosheets remain inactive under the same conditions.This study offers new strategies for rational design of carbon-based materials for solar-to-chemical energy conversion.
文摘Mesenchymal stem cells(MSCs)possess unique properties such as immunomodu-lation,paracrine actions,multilineage differentiation,and self-renewal.Therefore,MSC-based cell therapy is an innovative approach to treating various degenera-tive illnesses,including cardiovascular diseases.However,several challenges,including low transplant survival rates,low migration to the ischemic myocar-dium,and poor tissue retention,restrict the application of MSCs in clinical settings.These undesirable cell therapy outcomes mainly originated due to the overproduction of reactive oxygen species(ROS)in the injured heart.MSCs'stress-coping capacity can be enhanced by preconditioning them under conditions similar to the microenvironment of wounded tissues.Hydrogen peroxide(H_(2)O_(2))is a ROS that has been shown to activate protective cellular mechanisms such as survival,proliferation,migration,paracrine effects,and differentiation at suble-thal doses.These processes are induced via phosphatidylinositol 3-kinase/protein kinase B,p38 mitogen-activated protein kinases,c-Jun N-terminal kinase,Janus kinase/signal transducer and activator of the transcription,Notch1,and Wnt sig-naling pathways.H_(2)O_(2) preconditioning could lead to many clinical benefits,including ischemic injury reduction,enhanced survival of cellular transplants,and tissue regeneration.In this review,we present an overview of stem cell preconditioning methods and the biological functions activated by H_(2)O_(2) precondi-tioning.Furthermore,this review explores the molecular mechanisms underlying the protective cellular functions stimulated under H_(2)O_(2) preconditioning.
基金supported by the Korea Institute of Energy Technology Evaluation and Planning(KETEP)and the Ministry of Trade,Industry&Energy(MOTIE)of the Republic of Korea(no.20224000000020)supported by the MSIT(Ministry of Science and ICT),Korea,under the ICAN(ICT Challenge and Advanced Network of HRD)support program(IITP-2024-RS-2024-00437186)supervised by the IITP(Institute for Information&Communications Technology Planning&Evaluation)。
文摘Cobalt pentlandite(Co9S8)is a promising non-precious catalyst due to its superior oxygen reduction reaction activity and excellent stability.However,its oxygen reduction reaction catalytic activity has traditionally been limited to the four-electron pathway because of strong*OOH intermediate adsorption.In this study,we synthesized electron-deficient Co9S8 nanocrystals with an increased number of Co^(3+)states compared to conventional Co9S8.This was achieved by incorporating a high density of surface ligands in small-sized Co9S8nanocrystals,which enabled the transition of the electrochemical reduction pathway from four-electron oxygen reduction reaction to two-electron oxygen reduction reaction by decreasing*OOH adsorption strength.As a result,the Co^(3+)-enriched Co9S8 nanocrystals exhibited a high onset potential of 0.64 V(vs RHE)for two-electron oxygen reduction reaction,achieving H_(2)O_(2) selectivity of 70-80%over the potential range from 0.05 to 0.6 V.Additionally,these nanocrystals demonstrated a stable H_(2)O_(2) electrosynthesis at a rate of459.12 mmol g^(-1) h^(-1) with a H_(2)O_(2) Faradaic efficiency over 90%under alkaline conditions.This study provides insights into nanoscale catalyst design for modulating electrochemical reactions.
基金supported by the National Natural Science Foundation of China(Nos.22102073,22075147).
文摘As a versatile and environmentally benign oxidant,hydrogen peroxide(H_(2)O_(2))is highly desired in sanitation,disinfection,environmental remediation,and the chemical industry.Compared with the conventional anthraquinone process,the electrosynthesis of H_(2)O_(2)through the two-electron oxygen reduction reaction(2e^(−)ORR)is an efficient,competitive,and promising avenue.Electrocatalysts and devices are two core factors in 2e^(−)ORR,but the design principles of catalysts for different pH conditions and the development trends of relevant synthesis devices remain unclear.To this end,this review adopts a multiscale perspective to summarize recent advancements in the design principles,catalytic mechanisms,and application prospects of 2e^(−)ORR catalysts,with a particular focus on the influence of pH conditions,aiming at providing guidance for the selective design of advanced 2e^(−)ORR catalysts for highly-efficient H_(2)O_(2)production.Moreover,in response to diverse on-site application demands,we elaborate on the evolution of H_(2)O_(2)electrosynthesis devices,from rotating ring-disk electrodes and H-type cells to diverse flow-type cells.We elaborate on their characteristics and shortcomings,which can be beneficial for their further upgrades and customized applications.These insights may inspire the rational design of innovative catalysts and devices with high performance and wide serviceability for large-scale implementations.
基金supported by the National Natural Science Foundation of China (22209061 and 22462006)Start-up Fund for Senior Talents in Jiangsu University (21JDG060)the Fundamental Research Funds for the Central Universities (20720220009)
文摘Hydrogen peroxide(H_(2)O_(2))is an eco-friendly chemical with widespread industrial applications.However,the commercial anthraquinone process for H_(2)O_(2) production is energy-intensive and environmentally harmful,highlighting the need for more sustainable alternatives.The electrochemical production of H_(2)O_(2) via the two-electron water oxidation reaction(2e^(−)WOR)presents a promising route but is often hindered by low efficiency and selectivity,due to the competition with the oxygen evolution reaction.In this study,we employed high-throughput computational screening and microkinetic modeling to design a series of efficient 2e^(−)WOR electrocatalysts from a library of 240 single-metal-embedded nitrogen heterocycle aromatic molecules(M-NHAMs).These catalysts,primarily comprising post-transition metals,such as Cu,Ni,Zn,and Pd,exhibit high activity for H_(2)O_(2) conversion with a limiting potential approaching the optimal value of 1.76 V.Additionally,they exhibit excellent selectivity,with Faradaic efficiencies exceeding 80%at overpotentials below 300 mV.Structure-performance analysis reveals that the d-band center and magnetic moment of the metal center correlated strongly with the oxygen adsorption free energy(ΔGO*),suggesting these parameters as key catalytic descriptors for efficient screening and performance optimization.This study contributes to the rational design of highly efficient and selective electrocatalysts for electrochemical production of H_(2)O_(2),offering a sustainable solution for green energy and industrial applications.
基金Supported by Bozhou Key Research and Development Project,No.bzzc2020031.
文摘BACKGROUND Fistula-in-ano is an abnormal tunnel formation linking the anal canal with the perineum and perianal skin.Multiple imagining methods are available to evaluate it,among which magnetic resonance imaging(MRI)is the most advanced nonin-vasive preoperative method.However,it is limited in its visualization function.AIM To investigate the use of intraluminal MRI for perianal fistulas via a novel direct MRI fistulography method.METHODS We mixed 3%hydrogen peroxide(HP)with gadolinium for HPMRI fistulogra-phy,retrospectively analyzing 60 cases of complex/recurrent fistula-in-ano using physical examination,trans-perineal ultrasonography(TPUS),low-spatial-reso-lution MRI,and high-resolution direct HPMRI fistulography.We assessed detec-tion rates of fistula tracks,internal openings,their relationship with anal sphinc-ters,and perianal abscesses using statistical analyses,including interobserver agreement(Kappa statistic),and compared results with intraoperative findings.RESULTS Surgical confirmation in 60 cases showed that high-resolution direct HPMRI fis-tulography provided superior detection rates for internal openings(153)and fistula tracks(162)compared to physical exams,TPUS,and low-spatial-resolution MRI(Z>5.7,P<0.05).The effectiveness of physical examination and TPUS was also inferior to that of our method for detecting perianal abscesses(54)(Z=6.773,3.694,P<0.05),whereas that of low-spatial-resolution MRI was not significantly different(Z=1.851,P=0.06).High-resolution direct HPMRI fistulography also achieved the highest interobserver agreement(Kappa:0.89,0.85,and 0.80),while low-spatial-resolution MRI showed moderate agreement(Kappa:0.78,0.74,and 0.69).TPUS and physical examination had lower agreement(Kappa range:0.33-0.63).CONCLUSION High-resolution direct HPMRI fistulography enhances the visualization of recurrent and complex fistula-in-ano,including branched fistulas,allowing for precise planning and improved surgical outcomes.
文摘Photocatalytic hydrogen peroxide(H_(2)O_(2))production offers a sustainable route to convert water and oxygen into H_(2)O_(2)using solar energy.However,achieving long-term stability in photocatalysts remains a critical challenge due to mismatched kinetics between oxygen reduction(ORR)and water oxidation(WOR),which leads to hole accumulation and oxidative degradation.Here,we report a redox-mediated strategy to address this bottleneck by designing a hydroquinone-embedded covalent organic framework(Tz-QH-COF)that enables reversible hole buffering and kinetic balance.The hydroquinone(QH)units act as dynamic hole reservoirs,capturing excess holes during ORR and converting to benzoquinone(Q),which is regenerated to QH via WOR,thereby preventing oxidative decomposition.This reversible QH/Q cycle,directly visualized through in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy,ensures unmatched stability,achieving continuous H_(2)O_(2) production for 528 h(22 d)with an accumulated yield of 18.6 mmol L^(–1)—the highest reported duration for organic photocatalysts.Density functional theory calculations reveal that the QH units exhibit a strong oxygen adsorption energy and favorable two-electron ORR/WOR pathways with low energy barriers.The synergy between experimental and theoretical insights elucidates a redox-mediated charge-balance mechanism,advancing the design of robust photocatalysts for solar-driven H_(2)O_(2) synthesis.
基金supports from the National Natural Science Foundation of China(Nos.22478426 and 22278436)Young Elite Scientists Sponsorship Program by BAST(No.1101020370359)Science Foundation of China University of Petroleum,Beijing(No.2462021QNXZ009)。
文摘Advanced oxidation processes(AOPs)governed by peroxide activation to produce highly oxidative active species have been extensively explored for environmental remediation.Nevertheless,the low diffusion rates,inadequate interactions of the reactants,and limited active site exposure hinder treatment efficiency.Porous carbocatalysts with high specific surface area,tunable pore size,and programmable active sites demonstrate outstanding performance in activating diverse types of peroxides to generate active species for treatment of aqueous organic pollutants.The pore-rich structures enhance reaction kinetics for peroxide activation by facilitating diffusion of the reactants and their interactions.Additionally,the structural flexibility of porous structures favors the accommodation of highly dispersed metal species and allows for precise tuning of the microenvironment around the active sites,which further enhances the catalytic activity.This review critically summarizes the recent research progress in the applications of engineered porous carbocatalysts for peroxide activation and outlines the prevailing pore construction methods in carbocatalysts.Moreover,engineering strategies to regulate the mass transfer efficiency and fine-tune the microenvironment around the active sites are systematically addressed to enhance their catalytic peroxide activation performances.Challenges and future research opportunities pertaining to the design,optimization,mechanistic investigation,and practical application of porous carbocatalysts in peroxide activation are also proposed.
基金Supported by the Joint Logistics Support Force Comprehensive Equipment Research Project,No.LB2023B010100-09.
文摘BACKGROUND Current disinfection methods for gastrointestinal endoscopes consume a significant amount of water resources and produce a large volume of waste.AIM To achieve the objectives of efficiency,speed,and cost-effectiveness,this study utilized vaporized hydrogen peroxide(VHP)generated from sodium percarbonate granules to conduct an anhydrous disinfection test on gastrointestinal endoscopes.METHODS The experimental device rapidly converts sodium percarbonate granules into VHP,and performs disinfection experiments on gastrointestinal endoscope models,disposable endoscopes,and various types of reusable gastrointestinal endoscopes.Variables such as the intraluminal flow rate(FR),relative humidity(RH),exposure dosage,and organic burden are used to explore the factors influencing the disinfection of long and narrow lumens with VHP.RESULTS The device generates a certain concentration of VHP that can achieve high-level disinfection of endoscope models within 30 minutes.RH,exposure dosage,and organic burden significantly affect the disinfection efficacy of VHP,whereas the intraluminal FR does not significantly impact disinfection efficacy.All ten artificially contaminated disposable endoscopes achieved satisfactory disinfection results.Furthermore,when this device was used to treat various types of reusable endoscopes,the disinfection and sterilization effects were not significantly different from those of automatic endoscope disinfection machines(using peracetic acid disinfectant solution)(P>0.05),and the economic cost of disinfectant required per endoscope was lower(1.5 China Yuan),with a shorter disinfection time(30 minutes).CONCLUSION The methods and results of this study provide a basis for further research on the use of VHP for the disinfection of gastrointestinal endoscopes,as well as for the development of anhydrous disinfection technology for gastrointestinal endoscopes.
文摘In this editorial,a commentary on the article by Chang et al has been provided,the course of treatment of anorectal fistulas,especially complex and recurring ones,require accurate diagnostic procedures for determining ideal surgical procedures.Conventional ways of imaging sometimes fall short,offering insufficient insights in aggravated instances.In this editorial,a novel application of hydrogen peroxide-enhanced magnetic resonance imaging(HP-MRI)that promises significant improvements in the imaging of anorectal fistula.Study is based on a retrospective investigation of 60 patients,contrasts the new HP-MRI with conventional diagnostic techniques such as physical examination,trans-perineal ultrasonography and poor spatial resolution MRI.The findings demonstrate HP-MRI's incredible diagnostic performance,with sensitivity and specificity rates of 96.08%and 90.91%,respectively,and unparalleled interobserver agreement(Kappa values ranging from 0.80 to 0.89).It has been a significant advancement for assessment of anorectal fistulas providing a better roadmap for surgical planning,lowering recurrence rates as well as reduced personal and financial burden on patients by reducing the need for repeated treatment and extended hospital stays.The remaining funds can be utilized for treatment of other medical need.Ultimately HP-MRI provides us a healthier&more efficient society by improvising patients well-being&optimized healthcare infrastructure.
基金jointly supported by the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDB0750200)the National Key Research and Development Program of China(No.2023YFC3706600)the National Natural Science Foundation of China(Nos.22225605 and 22193051).
文摘Photocatalytic production of hydrogen peroxide(H_(2)O_(2))presents a promising strategy for environmental remediation and energy production.However,achieving clean and efficient H_(2)O_(2) production under ambient conditions without organic sacrificial agents remains challenging.Enhancing the low crystallinity of covalent organic frameworks(COFs)can promote the separation and transmission of photo-generated carriers,thereby boosting their photocatalytic performance.Herein,we introduce a novel synthetic approach by substituting traditional acetic acid catalysts with organic base catalysts to enhance the crystallinity of β-ketoenamine-linked COF,TpBD-COF.Compared to TpBD-COF-A synthesized using acetic acid catalysts,TpBD-COF-B,synthesized with organic base catalysts,exhibited advancements including increased absorption intensity in the visible spectrum,reduced photoluminescence intensity,enhanced photo-generated carrier separation performance,and a 2.1-fold increase in photocatalytic H_(2)O_(2) production.Under visible light irradiation,TpBDCOF-B achieved a photocatalytic H_(2)O_(2) production rate of 533μmol/h/g using only air and water,without the need for organic sacrificial agents.Furthermore,TpBD-COF-B also exhibited good performance in long-term catalytic production experiments,tests with actual water bodies,and cyclic usage experiments.This study offers a strategy for enhancing the crystallinity of COFs to improve their photocatalytic activity,with promising applications in clean energy production and environmental remediation.
基金financially supported by the National Natu-ral Science Foundation of China(Nos.21805052 and 22227804)the Guangdong Basic and Applied Basic Research Foundation(No.2023B1515020110)+4 种基金the Science and Technology Research Project of Guangzhou(Nos.202102020787 and 2023A03J0030)the De-partment of Science&Technology of Guangdong Province(No.2022A156)the Key Laboratory of Optoelectronic Materials and Sensors in Guangdong Provincial Universities(No.2023KSYS008)the Key Discipline of Materials Science and Engineering,Bureau of Education of Guangzhou(No.20225546)the College Student Innovation and Entrepreneurship Training Program of Guangzhou University(No.XJ202311078029).
文摘Selective electrocatalysis of two-electron oxygen reduction reaction(2e^(-)ORR)has been recognized as a sustainable and on-site process for hydrogen peroxide(H_(2)O_(2))production.Great progress has been achieved for 2e^(-)ORR in alkaline media.However,it is challenged by insufficient activity and selectiv-ity of the catalysts in acidic electrolytes.Herein,we report sulfur-poisoned PtNi/C catalysts(PtNiSx/C)that could regulate ORR from the 4e^(-)to 2e^(-)pathway.The identified PtNiS0.6/C offers high activity in terms of onset potential of∼0.69 V(vs.RHE)and∼80%selectivity.The mass activity is also compara-ble and outperforms representative Pt-based precious and transition-metal-based catalysts.In addition,it is interestingly found that the Faradaic efficiency further increased to 95%during the long-term elec-trolysis test due to Ni atom surface migration.The electrochemical production of the H_(2)O_(2)system was applied to the electro-Fenton process,which has realized the effective degradation of organic pollutants.This work offers a strategy by sulfur poisoning PtNi/C catalyst to realize Pt-based 2e^(-)ORR active catalysts to electrolysis of H_(2)O_(2)in acidic media.
基金supported by the National Natural Science Foundation of China(Nos.42077185,U22A20591)the Sichuan Science and Technology Program for Distinguished Young Scholars(Nos.2022JDJQ0010,2022ZYD0040)+1 种基金the National Key Research and Development Program of China(No.2020YFC1808300)the Research Fund of State Key Laboratory of Geohazard Prevention and Geoenvironment Protection(No.SKLGP2020Z002)。
文摘Degradation of nitrobenzene(NB)via Fenton-like reaction is considered as an efficient approach for contaminated groundwater remediation.However,the poor stability of H2O2limits the application of traditional Fenton reactions in soil and groundwater due to the transportation risks of H_(2)O_(2).In this study,we synthesized a controlled release nano calcium peroxide(n CP)by coating it with polydopamine(PDA)as a solid H2O2to construct a Fe(Ⅱ)/PDA@n CP Fenton-like system for contaminants degradation.The phenolquinone transformations of catechol groups on the PDA surface facilitated the Fe(Ⅱ)/Fe(Ⅲ)cycle,resulting in enhanced generation of hydroxyl radicals(HO·)and effective long-term degradation of NB.Moreover,the PDA shell modulated the n CP decomposition rate and inhibited sharp p H fluctuations,and the NB removal efficiency was achieved up to 96.8%at p H ranging from 3.0 to 9.0.This study demonstrated the promising application potential of PDA@n CP as a solid-controlled release H2O2source in Fenton-like system for groundwater contamination remediation.
基金financial support from the National Natural Science Foundation of China(No.22279143).
文摘Hydrogen peroxide(H_(2)O_(2))is a crucial,eco-friendly oxidizing agent with a wide range of industrial,environmental,and biomedical applications.Traditional production methods,such as the anthraquinone process,face significant challenges in terms of energy consumption and environmental impact.As a sustainable alternative,photocatalytic H_(2)O_(2) production,driven by solar energy,has emerged as a promising approach.This review discusses the key advancements in photocatalytic H_(2)O_(2) synthesis,focusing on overcoming challenges such as charge recombination,selectivity for the two-electron oxygen reduction reaction(2e^(-)ORR),and catalyst stability.Recent innovations in photocatalyst design,including high-entropy materials,single-atom catalysts,and covalent organic frameworks(COFs),have significantly enhanced efficiency and stability.Furthermore,novel strategies for optimizing charge separation,light harvesting,and mass transfer are explored.The integration of artificial intelligence and bioinspired systems holds potential for accelerating progress in this field.This review provides a comprehensive overview of current challenges and cutting-edge solutions,offering valuable insights for the development of scalable,decentralized H_(2)O_(2) production systems that contribute to a more sustainable future.
基金supported by the National Natural Science Foundation of China (29792072, 22278441, 22478452)National Key Research and Development Program of China (937) (2006CB202508)the SINOPEC Project (419019-2, 413108)。
文摘Propylene oxide(PO),with its reactive three-membered epoxide functional group,exhibits remarkable functional versatility and serves as a crucial bridge connecting the gaps between fossil energy utilization and chemical intermediate generation for new material innovation [1].For instance,PO's downstream derivatives,such as polyether polyols,carbonic esters,and polyurethanes,are widely utilized in wind power generation,battery electrolytes,solar cells,and CO_(2)-based degradable polymers,contributing to sustainable decarbonization in industry [2].
基金supported by the National Ten Thousand Talents Plan and the high-performance computing platform of Guizhou Universitythe Program of Introducing Talents to Chinese Universities(no.D20023)+1 种基金the Central Government Guides Local Science and Technology Development Fund Projects(Qiankehezhongyindi(2023)001)the Frontiers Science Centre for Asymmetric Synthesis and Medicinal Molecules,and the Department of Education,Guizhou Province[Qianjiaohe KY(2020)004].
文摘Photocatalytic technology has attracted much attention in the fields of clean energy and environmental governance.However,how to design and develop highly efficient photocatalytic materials remains an urgent scientific problem to be solved.This study focuses on enhancing photocatalytic activity through microstructure modification.Among them,ToRed-4 showed the most prominent performance.Under the illumination condition of 420 nm,its value was 13506 lmol g^(-1) h^(-1),which was approximately 18 times that of CN550(bulk g-C_(3)N_(4))(719 lmol g^(-1) h^(-1)).By using DFT calculations,the photocatalytic performance was deeply analyzed,revealing the significant advantages of the ToRed series in key performance indicators and the underlying synergy mechanisms,including the reduction of the HOMO-LUMO energy gap,the efficient separation of electron holes,the expansion of the electronic transition range,the transformation of the electrostatic potential distribution,the increase in dipole moment,and the optimization of the Coulomb attractive energy.The research results of this study provide a key basis for opening up new avenues for the design and development of highly efficient photocatalytic materials and are expected to play an important role in related fields.
