Photosynthesis of H_(2)O_(2)via sustainable biomass-derived carbon catalysts facilitate the conversion of renewable resources into valuable chemicals.However,the regulatory function of surface functional groups over r...Photosynthesis of H_(2)O_(2)via sustainable biomass-derived carbon catalysts facilitate the conversion of renewable resources into valuable chemicals.However,the regulatory function of surface functional groups over reaction kinetics has not been sufficiently investigated.Herein,hydrothermal carbon spheres(CS)rich in oxygencontaining functional groups demonstrated a remarkably high H_(2)O_(2)production rate(653μmol/(g·h))in both pure water and actual seawater,even in the absence of any sacrificial agent.Meanwhile,the catalyst demonstrates outstanding activity(92%conversion and>99%selectivity)in the visible-light-driven photocatalytic oxidation of benzylamine to imines.Comprehensive analysis reveals that CS was rich in surface oxygen-containing functional groups,a feature strongly associated with its high photocatalytic efficiency.The observed positive Zeta potential of CS in seawater likely diminished the electrostatic repulsion against the positively charged intermediates,thereby facilitating their accumulation at the liquid-solid interface.This work proposes a strategic framework for developing metal-free photocatalysts from biomass,offering a sustainable pathway for photocatalytic applications.展开更多
Lithium-ion capacitors(LICs)combine the high power dens-ity of electrical double-layer capacitors with the high energy density of lithium-ion batteries.However,they face practical limitations due to the narrow operati...Lithium-ion capacitors(LICs)combine the high power dens-ity of electrical double-layer capacitors with the high energy density of lithium-ion batteries.However,they face practical limitations due to the narrow operating voltage window of their activated carbon(AC)cathodes.We report a scalable thermal treatment strategy to develop high-voltage-tolerant AC cathodes.Through controlled thermal treatment of commer-cial activated carbon(Raw-AC)under a H_(2)/Ar atmosphere at 400-800℃,the targeted reduction of degradation-prone functional groups can be achieved while preserving the critical pore structure and increasing graph-itic microcrystalline ordering.The AC treated at 400℃(HAC-400)had a significant increase in specific capacity(96.0 vs.75.1 mAh/g at 0.05 A/g)and better rate capability(61.1 vs.36.1 mAh/g at 5 A/g)in half-cell LICs,along with an 83.5%capacity retention over 7400 cycles within an extended voltage range of 2.0-4.2 V in full-cell LICs.Scalability was demonstrated by a 120 g batch production,enabling fabrication of pouch-type LICs with commercial hard carbon anodes that delivered a higher energy density of 28.3 Wh/kg at 1 C,and a peak power density of 12.1 kW/kg compared to devices using raw AC.This simple,industry-compatible approach may be used for producing ad-vanced cathode materials for practical high-performance LICs.展开更多
Biochar(BC)are widely used as highly efficient adsorbents to alleviate aromatics-based contaminants due to their ease of preparation,wide availability,and high sustainability.The surface properties of BCs usually vary...Biochar(BC)are widely used as highly efficient adsorbents to alleviate aromatics-based contaminants due to their ease of preparation,wide availability,and high sustainability.The surface properties of BCs usually vary greatly due to their complex chemical constituents and different preparation processes and are reflected in the values of parameters such as the specific surface area(SSA),pore volume/size,and surface functional groups(SFGs).The effects of SSA and pore volume/size on the adsorption of aromatics have been widely reported.However,the corresponding mechanisms of BC SFGs towards aromatics adsorption remains unclear as the compositions of the SFGs are usually complex and hard to determine.To address in this gap in the literature,this review introduces a new perspective on the adsorption mechanisms of aromatics.Through collecting previously-reported results,the parameters log P(logarithm of the Kow),polar surface area,and the positive/negative charges were carefully calculated using Chem Draw3D,which allowed the hydrophobicity/hydrophilicity properties,electron donor-acceptor interactions,Hbonding,and electrostatic interactions between SFGs and aromatics-based contaminates to be inferred intuitively.These predictions were consistent with the reported results and showed that tailor-made BCs can be designed according to the molecular weights,chemical structures,and polarities of the target aromatics.Overall,this review provides new insight into predicting the physicochemical properties of BCs through revealing the relationship between SFGs and adsorbates,which may provide useful guidance for the preparing of highly-efficient,functional BCs for the adsorption of aromatics.展开更多
The activated carbon with high surface area was prepared by KOH activation.It was further modified by H2SO4 and HNO3 to introduce more surface functional groups.The pore structure of the activated carbons before and a...The activated carbon with high surface area was prepared by KOH activation.It was further modified by H2SO4 and HNO3 to introduce more surface functional groups.The pore structure of the activated carbons before and after modification was analyzed based on the nitrogen adsorption isotherms.The morphology of those activated carbons was characterized using scanning electronic microscopy （SEM）.The surface functional groups were determined by Fourier transform infrared spectroscopy （FTIR）.The quantity of those groups was measured by the Boehm titration method.Cr（VI） removal by the activated carbons from aqueous solution was investigated at different pH values.The results show that compared with H2SO4,HNO3 destructs the original pore of the activated carbon more seriously and induces more acidic surface functional groups on the activated carbon.The pH value of the solution plays a key role in the Cr（VI） removal.The ability of reducing Cr（VI） to Cr（III） by the activated carbons is relative to the acidic surface functional groups.At higher pH values,the Cr（VI） removal ratio is improved by increasing the acidic surface functional groups of the activated carbons.At lower pH values,however,the acidic surface functional groups almost have no effect on the Cr（VI） removal by the activated carbon from aqueous solution.展开更多
The thermal deactivation of diesel soot particles exerts a significant influence on the control strategy for the regeneration of diesel particulate filters(DPFs).This work focused on the changes in the surface functio...The thermal deactivation of diesel soot particles exerts a significant influence on the control strategy for the regeneration of diesel particulate filters(DPFs).This work focused on the changes in the surface functional groups,carbon chemical state,and graphitization degree during thermal treatment in an inert gas environment at intermediate temperatures of 600℃,800℃,and 1000℃ and explore the chemical species that were desorbed from the diesel soot surface during thermal treatment using a thermogravimetric analyser coupled with a gas-chromatograph mass spectrometer(TGA-GC/MS).The surface functional groups and carbon chemical statewere characterized using Fourier transform infrared spectroscopy(FT-IR)and X-ray photoelectron spectroscopy(XPS).The graphitization degree was evaluated by means of Raman spectroscopy(RS).The concentrations of aliphatic C–H,C–OH,C=O,and O–C=O groups are reduced for diesel soot and carbon black when increasing the thermal treatment temperature,while the sp^(2)/sp^(3) hybridized ratio and graphitization degree enhance.These results provide comprehensive evidence of the decreased reactivity of soot samples.Among oxygenated functional groups,the percentage reduction during thermal treatment is the largest for the O–C=O groups owing to its worst thermodynamic stability.TGA-GC/MS results show that the aliphatic and aromatic chains and oxygenated species would be desorbed from the soot surface during 1000℃ thermal treatment of diesel soot.展开更多
The functional groups on graphene sheets surface affect their dispersion and interfacial adhesion in polymer matrix. We compared the mechanical property of polymethymethacrylate（PMMA） microcellular foams reinforced ...The functional groups on graphene sheets surface affect their dispersion and interfacial adhesion in polymer matrix. We compared the mechanical property of polymethymethacrylate（PMMA） microcellular foams reinforced with graphene oxide（GO） and reduced graphene oxide（RGO） to investigate this influence of functional groups. RGO sheets were fabricated by solvent thermal reduction in DMF medium. UV-Vis, FT-IR and XPS analyses indicate the difference of oxygen-containing groups on GO and RGO sheets surface. The observation of SEM illustrates that the addition of a smaller number of GO or RGO sheets causes a fine cellular structure of PMMA foams with a higher cell density(about 1011 cells/cm3) and smaller cell sizes（about 1-2 μm） owing to their remarkable heterogeneous nucleation effect. Compared to GO reinforced foams, the RGO/PMMA foams own lower cell density and bigger cell size in their microstructure, and their compressive strength is lower even when the reinforcement contents are the same and the foam bulk density is higher. These results indicate that the oxygen-containing groups on GO sheets’ surface are beneficial to adhere CO2 to realize a larger nucleation rate, and their strong interaction with PMMA matrix improves the mechanical property of PMMA foams.展开更多
Water pollution regarding dyes and heavy metal ions is crucial facing the world.How to effectively separate these contaminants from water has been a key issue.Graphene oxide(GO)promises the greenwater world as a long-...Water pollution regarding dyes and heavy metal ions is crucial facing the world.How to effectively separate these contaminants from water has been a key issue.Graphene oxide(GO)promises the greenwater world as a long-lasting spotlight adsorbent material and therefore,harnessing GO has been the research hotspot for over a decade.The state of GO as well as its surface functional groups plays an important role in adsorption.And the way of preparation and structural modification matters to the performance of GO.In this review,the significance of the state of existence of stock GO and surface functional groups is explored in terms of preparation,structural modification,and adsorption.Besides,various adsorbates for GO adsorption are also involved,the discussion of which is rarely established elsewhere.展开更多
FeO;supported on activated carbon(AC) has been shown to be an ideal catalyst for catalytic wet peroxide oxidation(CWPO) due to its high CWPO reaction activity and stability. Although there have been some studies on th...FeO;supported on activated carbon(AC) has been shown to be an ideal catalyst for catalytic wet peroxide oxidation(CWPO) due to its high CWPO reaction activity and stability. Although there have been some studies on the mechanism of Fe/AC catalysis in CWPO, the specific contribution of each component(surface oxygen groups and FeOxon AC) inside an Fe/AC catalyst and their corresponding reaction mechanism remain unclear, and the reaction stability of CWPO catalysts has rarely been discussed. Then the optimal CWPO catalyst in our laboratory, 3%Fe/AC, was selected.(1) By removing certain components on the AC through heat treatment, its contribution to the reaction and the corresponding reaction mechanism were investigated. With the aid of temperature-programmed desorption–mass spectrometry(TPD–MS) and the CWPO reaction, the normalized catalytic contributions of components were shown to be: 37.3%(carboxylic groups), 5.3%(anhydride), 19.3%(ether/hydroxyl),-71.4%(carbonyl groups) and 100%(FeOx),respectively. DFT calculation and EPR analysis confirmed that carboxylic groups and Fe_(2)O_(3) are able to activate the H_(2)O_(2) to generate·OH.(2) The catalysts at were characterized at different reaction times(0 h, 450 h, 900 h, 1350 h, and 1800 h) by TPD–MS and M?ssbauer spectroscopy. Results suggested that the number of carboxylic goups gradually increased and the size of paramagnetic Fe_(2)O_(3) particle crystallites gradually increased as the reactions progressed. The occurrence of strong interactions between metal oxides and AC was also confirmed. Due to these effects, the strong stability of 3%Fe/AC was further improved. Therefore, the reasons for the high activity and strong stability of 3%Fe/AC in CWPO were clearly shown. We believe that this work provides an idea of the removal of cresols from wastewater into the introduction to show the potential applications of CWPO.展开更多
A series of activated carbons（ACs） were prepared using HNO_3,H_2O_2 and steam as activation agents with the aim to introduce functional groups to carbon surface in the ACs preparation process.The effects of concentr...A series of activated carbons（ACs） were prepared using HNO_3,H_2O_2 and steam as activation agents with the aim to introduce functional groups to carbon surface in the ACs preparation process.The effects of concentration of activation agent,activation time on the surface functional groups and redox property of ACs were characterized by Temperature Program Desorption（TPD） and Cyclic Voltammetry（CV）.Results showed that lactone groups of ACs activated by HNO_3 increase with activation time,and the carboxyl groups increase with the concentration of HNO_3.Carbonyl/quinine groups of ACs activated by H_2O_2 increase with the activation time and the concentration of H_2O_2,although the acidic groups decrease with the concentration of H_2O_2.The redox property reflected by CV at 0 and 0.5 V is different with any kinds of oxygen functional groups characterized by TPD,but it is consistent with the SO_2 catalytic oxidization /oxidation properties indicated by TPR.展开更多
During the initial impoundment period of a canyon-shaped reservoir,the water body fluctuated violently regarding water level,hydrological condition,and thermal stratification.These variations may alter the structure o...During the initial impoundment period of a canyon-shaped reservoir,the water body fluctuated violently regarding water level,hydrological condition,and thermal stratification.These variations may alter the structure of phytoplankton community,resulting in algal blooms and seriously threatening the ecological security of the reservoir.It is of great significance to understand the continuous changes of phytoplankton in the initial impoundment period for the protection of reservoir water quality.Therefore,a two-year in-situ monitoring study was conducted on water quality and phytoplankton in a representative canyonshaped reservoir named Sanhekou and the interannual changes of phytoplankton community and its response to environmental changes during the initial impoundment period were discussed at taxonomic versus functional classification levels.The results showed that the total nitrogen and permanganate index levels were relatively high in the first year due to rapid water storage and heavy rainfall input,and the more stable hydrological conditions in the second year promoted the increase of algae density and the transformation of community,and the proportion of cyanobacteria increased significantly.The succession order of phytoplankton in the first year of the initial impoundment periodwas Chlorophyta-Bacillariophyta-Chlorophyta,or J/F/X1-P/MP/W1-A/X1/MP,respectively.And the succession order in the second year was Cyanobacteria/Chlorophyta-Bacillariophyta-Chlorophyta,or L_(M)/G/P-P/A/X1-X1/J/G.Water temperature,relativewater column stability,mixing depth,and pHwere crucial factors affecting phytoplankton community succession.This study revealed the interannual succession law and driving factors of phytoplankton in the initial impoundment period and provided an important reference for the operation management and ecological protection of canyon-shaped reservoirs.展开更多
Bacterial surface glycans perform a diverse and important set of biological roles,and have been widely used in the treatment of bacterial infectious diseases.The majority of bacterial surface glycans are decorated wit...Bacterial surface glycans perform a diverse and important set of biological roles,and have been widely used in the treatment of bacterial infectious diseases.The majority of bacterial surface glycans are decorated with diverse rare functional groups,including amido,acetamidino,carboxamido and pyruvate groups.These functional groups are thought to be important constituents for the biological activities of glycans.Chemical synthesis of glycans bearing these functional groups or their variants is essential for the investigation of structure-activity relationships by a medicinal chemistry approach.To date,a broad choice of synthetic methods is available for targeting the different rare functional groups in bacterial surface glycans.This article reviews the structures of naturally occurring rare functional groups in bacterial surface glycans,and the chemical methods used for installation of these groups.展开更多
In this work,a modification method of H_(3)PO_(4)plus H_(2)O_(2)(PHP)was introduced to targetedly form abundant oxygenated functional groups(OFGs)on biochar,and methylene blue(MB)was employed as a model pollutant for ...In this work,a modification method of H_(3)PO_(4)plus H_(2)O_(2)(PHP)was introduced to targetedly form abundant oxygenated functional groups(OFGs)on biochar,and methylene blue(MB)was employed as a model pollutant for adsorption to reflect the modification performance.Results indicated that parent biochars,especially derived from lower temperatures,substantially underwent oxidative modification by PHP,and OFGs were targetedly produced.Correspondingly,approximately 21.5-fold MB adsorption capacity was achieved by PHP-modified biochar comparing with its parent biochar.To evaluate the compatibility of PHP-modification,coefficient of variation(CV)based on MB adsorption capacity by the biochar from various precursors was calculated,in which the CV of PHP-modified biochars was 0.0038 comparing to0.64 of the corresponding parent biochars.These results suggested that the PHP method displayed the excellent feedstock compatibility on biochar modification.The maximum MB adsorption capacity was454.1 mg/g when the H_(3)PO_(4)and H_(2)O_(2)fraction in PHP were 65.2%and 7.0%;the modification was further intensified by promoting temperature and duration.Besides,average 94.5%H_(3)PO_(4)was recovered after 10-batch modification,implying 1.0 kg H_(3)PO_(4)(85%)in PHP can maximally modify 2.37 kg biochar.Overall,this work offered a novel method to tailor biochar towards OFGs-rich surface for efficient adsorption.展开更多
The industrial silica fume pretreated by nitric acid at 80 °C was re-used in this work. Then, the obtained silica nanoparticles were surface functionalized by silane coupling agents, such as(3-Mercaptopropyl) tri...The industrial silica fume pretreated by nitric acid at 80 °C was re-used in this work. Then, the obtained silica nanoparticles were surface functionalized by silane coupling agents, such as(3-Mercaptopropyl) triethoxysilane(MPTES) and(3-Amincpropyl) trithoxysilane(APTES). Some further modifications were studied by chloroaceetyl choride and 1,8-Diaminoaphalene for amino modified silica. The surface functionalized silica nanoparticles were characterized by Fourier transform infrared(FI-IR) and X-ray photoelectron spectroscopy(XPS). The prepared adsorbent of surface functionalized silica nanoparticles with differential function groups were investigated in the selective adsorption about Pb2+, Cu2+, Hg2+, Cd2+ and Zn2+ions in aqueous solutions. The results show that the(3-Mercaptopropyl) triethoxysilane functionalized silica nanoparticles(SiO2-MPTES) play an important role in the selective adsorption of Cu2+ and Hg2+, the(3-Amincpropyl) trithoxysilane(APTES) functionalized silica nanoparticles(SiO2-APTES) exhibited maximum removal efficiency towards Pb2+ and Hg2+, the 1,8-Diaminoaphalene functionalized silica nanoparticles was excellent for removal of Hg2+ at room temperature, respectively.展开更多
Hydrogel scaffolds have numerous potential applications in the tissue engineering field.However,tough hydrogel scaffolds implanted in vivo are seldom reported because it is difficult to balance biocompatibility and hi...Hydrogel scaffolds have numerous potential applications in the tissue engineering field.However,tough hydrogel scaffolds implanted in vivo are seldom reported because it is difficult to balance biocompatibility and high mechanical properties.Inspired by Chinese ramen,we propose a universal fabricating method(printing-P,training-T,cross-linking-C,PTC&PCT)for tough hydrogel scaffolds to fill this gap.First,3D printing fabricates a hydrogel scaffold with desired structures(P).Then,the scaffold could have extraordinarily high mechanical properties and functional surface structure by cycle mechanical training with salting-out assistance(T).Finally,the training results are fixed by photo-cross-linking processing(C).The tough gelatin hydrogel scaffolds exhibit excellent tensile strength of 6.66 MPa(622-fold untreated)and have excellent biocompatibility.Furthermore,this scaffold possesses functional surface structures from nanometer to micron to millimeter,which can efficiently induce directional cell growth.Interestingly,this strategy can produce bionic human tissue with mechanical properties of 10 kPa-10 MPa by changing the type of salt,and many hydrogels,such as gelatin and silk,could be improved with PTC or PCT strategies.Animal experiments show that this scaffold can effectively promote the new generation of muscle fibers,blood vessels,and nerves within 4 weeks,prompting the rapid regeneration of large-volume muscle loss injuries.展开更多
To prepare a highly efficient NiMo/Al_(2)O_(3) hydrodesulfurization catalyst,the combined effects of specific organic functional groups and alumina surface characteristics were investigated.First,the correlation betwe...To prepare a highly efficient NiMo/Al_(2)O_(3) hydrodesulfurization catalyst,the combined effects of specific organic functional groups and alumina surface characteristics were investigated.First,the correlation between the surface characteristics of four different alumina and the existing Mo species states was established.It was found that the Mo equilibrium adsorption capacity can be used as a specific descriptor to quantitatively evaluate the changes in surface characteristics of different alumina.A lower Mo equilibrium adsorption capacity for alumina means weaker metal-support interaction and the loaded Mo species are easier to transform into MoS2.However,the Mo-O-Al bonds still exist at the metal-support interface.The introduction of cationic surfactant hecadecyl trimethyl ammonium bromide(CTAB)can further improve Mo species dispersion through electrostatic attraction with Mo anions and interaction of its alkyl chain with the alumina surface;meanwhile,the introduction of ethylenediamine tetraacetic acid(EDTA)can complex with Ni ions to enhance the Ni-promoting effect on Mo.Therefore,the NiMo catalyst designed using alumina with lower Mo equilibrium adsorption capacity and the simultaneous addition of EDTA and CTAB exhibits the highest hydrodesulfurization activity for 4,6-dimethyl dibenzothiophene because of its proper metal-support interaction and more well-dispersed Ni-Mo-S active phases.展开更多
As a new electrochemical technology,capacitive deionization(CDI)has been increasingly applied in environmental water treatment and seawater desalination.In this study,functional groups modified porous hollow carbon(HC...As a new electrochemical technology,capacitive deionization(CDI)has been increasingly applied in environmental water treatment and seawater desalination.In this study,functional groups modified porous hollow carbon(HC)were synthesized as CDI electrode material for removing Na^(+)and Cl^(−)in salty water.Results showed that the average diameter of HC was approximately 180 nm,and the infrared spectrum showed that its surface was successfully modified with sulfonic and amino groups,respectively.The sulfonic acid functionalized HC(HC-S)showed better electrochemical and desalting performance than the amino-functionalized HC(HC–N),with a maximum Faradic capacity of 287.4 F/g and an adsorptive capacity of 112.97 mg/g for NaCl.Additionally,92.63%capacity retention after 100 adsorption/desorption cycles demonstrates the excellent stability of HC-S.The main findings prove that HC-S is viable as an electrodematerial for desalination by high-performance CDI applications.展开更多
Magnetically responsive microstructured functional surface(MRMFS),capable of dynamically and reversibly switching the surface topography under magnetic actuation,provides a wireless,noninvasive,and instantaneous way t...Magnetically responsive microstructured functional surface(MRMFS),capable of dynamically and reversibly switching the surface topography under magnetic actuation,provides a wireless,noninvasive,and instantaneous way to accurately control the microscale engineered surface.In the last decade,many studies have been conducted to design and optimize MRMFSs for diverse applications,and significant progress has been accomplished.This review comprehensively presents recent advancements and the potential prospects in MRMFSs.We first classify MRMFSs into one-dimensional linear array MRMFSs,two-dimensional planar array MRMFSs,and dynamic self-assembly MRMFSs based on their morphology.Subsequently,an overview of three deformation mechanisms,including magnetically actuated bending deformation,magnetically driven rotational deformation,and magnetically induced self-assembly deformation,are provided.Four main fabrication strategies employed to create MRMFSs are summarized,including replica molding,magnetization-induced self-assembly,laser cutting,and ferrofluid-infused method.Furthermore,the applications of MRMFS in droplet manipulation,solid transport,information encryption,light manipulation,triboelectric nanogenerators,and soft robotics are presented.Finally,the challenges that limit the practical applications of MRMFSs are discussed,and the future development of MRMFSs is proposed.展开更多
Rayon-based carbon fibers were anodically oxidized in the presence of a variety of electrolytes. The functional groups produced on carbon fiber surface were characterized by Fourier Transform Infrared Spectroscopy (FT...Rayon-based carbon fibers were anodically oxidized in the presence of a variety of electrolytes. The functional groups produced on carbon fiber surface were characterized by Fourier Transform Infrared Spectroscopy (FTIR). Both K Br pellet spectra and ATR difference spectra indicate that carboxyl and phenolic and carbonyl groups were produced. The acidic groups, carboxyl and phenol, were measured by potentiometrie titration with standard solutions of acid and alkali. The results show that the amount of acidic groups is related to the electrolyte used.展开更多
Taking the Lower Silurian Longmaxi Formation shale in the Sichuan Basin as an example,this study employs atomic force microscopy-based infrared(AFM-IR)spectroscopy to analyze the submicron-scale molecular functional g...Taking the Lower Silurian Longmaxi Formation shale in the Sichuan Basin as an example,this study employs atomic force microscopy-based infrared(AFM-IR)spectroscopy to analyze the submicron-scale molecular functional groups of different types and occurrences of organic matter.Combined with the quantitative evaluation of pore development via scanning electron microscopy(SEM),the response of organic pore formation and evolution mechanisms to chemical composition and structural evolution of organic matter in overmature marine shale is investigated.The results indicate that the AFM-IR spectra of graptolite periderms and pyrobitumen in shale are dominated by the stretching vibrations of conjugated C=C bonds in aromatic compounds at approximately 1600 cm-1,with weak absorption peaks near 1375,1450 and 1720 cm-1,corresponding to aliphatic chains and carbonyl/carboxyl functional groups.Overall,the AFM-IR structural indices(A and C factors)of organic matter show a strong correlation with visible porosity in shales of equivalent maturity.Lower A and C factor values correlate with enhanced development of organic pores,which is associated with the detachment of more aliphatic chains and oxygen-containing functional groups during thermal evolution.Pyrobitumen-clay mineral composites generally exhibit superior pore development,likely attributable to clay mineral dehydration participating in hydrocarbon generation reactions that promote the removal of more functional groups.Additionally,hydrocarbon generation within organic-clay composites during high-over mature stages may induce volumetric expansion,resulting in microfracturing and hydrocarbon expulsion.The associated higher hydrocarbon expulsion rates promote the formation of larger pores and fracture-shaped pores along the flake-shaped clay minerals.This study highlights that the research of submicron-scale molecular functional groups provides a deeper understanding of organic matter evolution and pores development mechanisms in overmature shales,thereby offering critical theoretical parameters for reservoir evaluation in shale oil and gas exploration.展开更多
Biomass-derived carbon materials are favored for their abundance and sustainability,and ease of preparation and modification.By surface activation and modification they can have a good electrical conductivity,excellen...Biomass-derived carbon materials are favored for their abundance and sustainability,and ease of preparation and modification.By surface activation and modification they can have a good electrical conductivity,excellent catalytic activity,a remarkable adsorption capacity,and different interfacial physicochemical functionalities.Surface-modified biochars have found wide applications in energy storage,environmental remediation,and catalysis.However,achieving precise and controllable modification of their active sites remains a challenge.Recent advances and future prospects for controlling their surface morphology,defect engineering,and surface coating strategies,with particular attention to their means of fabrication,are reviewed.展开更多
基金Supported by the Natural Science Foundation of Shanxi Province(202203021222233,202203021212398,202203021212403)。
文摘Photosynthesis of H_(2)O_(2)via sustainable biomass-derived carbon catalysts facilitate the conversion of renewable resources into valuable chemicals.However,the regulatory function of surface functional groups over reaction kinetics has not been sufficiently investigated.Herein,hydrothermal carbon spheres(CS)rich in oxygencontaining functional groups demonstrated a remarkably high H_(2)O_(2)production rate(653μmol/(g·h))in both pure water and actual seawater,even in the absence of any sacrificial agent.Meanwhile,the catalyst demonstrates outstanding activity(92%conversion and>99%selectivity)in the visible-light-driven photocatalytic oxidation of benzylamine to imines.Comprehensive analysis reveals that CS was rich in surface oxygen-containing functional groups,a feature strongly associated with its high photocatalytic efficiency.The observed positive Zeta potential of CS in seawater likely diminished the electrostatic repulsion against the positively charged intermediates,thereby facilitating their accumulation at the liquid-solid interface.This work proposes a strategic framework for developing metal-free photocatalysts from biomass,offering a sustainable pathway for photocatalytic applications.
文摘Lithium-ion capacitors(LICs)combine the high power dens-ity of electrical double-layer capacitors with the high energy density of lithium-ion batteries.However,they face practical limitations due to the narrow operating voltage window of their activated carbon(AC)cathodes.We report a scalable thermal treatment strategy to develop high-voltage-tolerant AC cathodes.Through controlled thermal treatment of commer-cial activated carbon(Raw-AC)under a H_(2)/Ar atmosphere at 400-800℃,the targeted reduction of degradation-prone functional groups can be achieved while preserving the critical pore structure and increasing graph-itic microcrystalline ordering.The AC treated at 400℃(HAC-400)had a significant increase in specific capacity(96.0 vs.75.1 mAh/g at 0.05 A/g)and better rate capability(61.1 vs.36.1 mAh/g at 5 A/g)in half-cell LICs,along with an 83.5%capacity retention over 7400 cycles within an extended voltage range of 2.0-4.2 V in full-cell LICs.Scalability was demonstrated by a 120 g batch production,enabling fabrication of pouch-type LICs with commercial hard carbon anodes that delivered a higher energy density of 28.3 Wh/kg at 1 C,and a peak power density of 12.1 kW/kg compared to devices using raw AC.This simple,industry-compatible approach may be used for producing ad-vanced cathode materials for practical high-performance LICs.
基金funded by the National Natural Science Foundation of China(No.51961165104)Project of Thousand Youth Talents(No.AUGA2160100917)+1 种基金University Nursing Program for Young Scholars with Creative Talents in Heilongjiang Province(No.UNPYSCT-2020050)Provincial Leading Talent Echelon Cultivation Project of Heilongjiang Institute of Technology(No.2020LJ04)。
文摘Biochar(BC)are widely used as highly efficient adsorbents to alleviate aromatics-based contaminants due to their ease of preparation,wide availability,and high sustainability.The surface properties of BCs usually vary greatly due to their complex chemical constituents and different preparation processes and are reflected in the values of parameters such as the specific surface area(SSA),pore volume/size,and surface functional groups(SFGs).The effects of SSA and pore volume/size on the adsorption of aromatics have been widely reported.However,the corresponding mechanisms of BC SFGs towards aromatics adsorption remains unclear as the compositions of the SFGs are usually complex and hard to determine.To address in this gap in the literature,this review introduces a new perspective on the adsorption mechanisms of aromatics.Through collecting previously-reported results,the parameters log P(logarithm of the Kow),polar surface area,and the positive/negative charges were carefully calculated using Chem Draw3D,which allowed the hydrophobicity/hydrophilicity properties,electron donor-acceptor interactions,Hbonding,and electrostatic interactions between SFGs and aromatics-based contaminates to be inferred intuitively.These predictions were consistent with the reported results and showed that tailor-made BCs can be designed according to the molecular weights,chemical structures,and polarities of the target aromatics.Overall,this review provides new insight into predicting the physicochemical properties of BCs through revealing the relationship between SFGs and adsorbates,which may provide useful guidance for the preparing of highly-efficient,functional BCs for the adsorption of aromatics.
文摘The activated carbon with high surface area was prepared by KOH activation.It was further modified by H2SO4 and HNO3 to introduce more surface functional groups.The pore structure of the activated carbons before and after modification was analyzed based on the nitrogen adsorption isotherms.The morphology of those activated carbons was characterized using scanning electronic microscopy （SEM）.The surface functional groups were determined by Fourier transform infrared spectroscopy （FTIR）.The quantity of those groups was measured by the Boehm titration method.Cr（VI） removal by the activated carbons from aqueous solution was investigated at different pH values.The results show that compared with H2SO4,HNO3 destructs the original pore of the activated carbon more seriously and induces more acidic surface functional groups on the activated carbon.The pH value of the solution plays a key role in the Cr（VI） removal.The ability of reducing Cr（VI） to Cr（III） by the activated carbons is relative to the acidic surface functional groups.At higher pH values,the Cr（VI） removal ratio is improved by increasing the acidic surface functional groups of the activated carbons.At lower pH values,however,the acidic surface functional groups almost have no effect on the Cr（VI） removal by the activated carbon from aqueous solution.
基金supported by the National Natural Science Foundation of China (No.52006054)the State Key Laboratory of Engines at Tianjin University (No.K2021-05)+1 种基金the European Union’s projects MODALES (No.815189)nPETS (No.954377)
文摘The thermal deactivation of diesel soot particles exerts a significant influence on the control strategy for the regeneration of diesel particulate filters(DPFs).This work focused on the changes in the surface functional groups,carbon chemical state,and graphitization degree during thermal treatment in an inert gas environment at intermediate temperatures of 600℃,800℃,and 1000℃ and explore the chemical species that were desorbed from the diesel soot surface during thermal treatment using a thermogravimetric analyser coupled with a gas-chromatograph mass spectrometer(TGA-GC/MS).The surface functional groups and carbon chemical statewere characterized using Fourier transform infrared spectroscopy(FT-IR)and X-ray photoelectron spectroscopy(XPS).The graphitization degree was evaluated by means of Raman spectroscopy(RS).The concentrations of aliphatic C–H,C–OH,C=O,and O–C=O groups are reduced for diesel soot and carbon black when increasing the thermal treatment temperature,while the sp^(2)/sp^(3) hybridized ratio and graphitization degree enhance.These results provide comprehensive evidence of the decreased reactivity of soot samples.Among oxygenated functional groups,the percentage reduction during thermal treatment is the largest for the O–C=O groups owing to its worst thermodynamic stability.TGA-GC/MS results show that the aliphatic and aromatic chains and oxygenated species would be desorbed from the soot surface during 1000℃ thermal treatment of diesel soot.
基金Funded by the National Nature Science Foundation of China(No.51521001)
文摘The functional groups on graphene sheets surface affect their dispersion and interfacial adhesion in polymer matrix. We compared the mechanical property of polymethymethacrylate（PMMA） microcellular foams reinforced with graphene oxide（GO） and reduced graphene oxide（RGO） to investigate this influence of functional groups. RGO sheets were fabricated by solvent thermal reduction in DMF medium. UV-Vis, FT-IR and XPS analyses indicate the difference of oxygen-containing groups on GO and RGO sheets surface. The observation of SEM illustrates that the addition of a smaller number of GO or RGO sheets causes a fine cellular structure of PMMA foams with a higher cell density(about 1011 cells/cm3) and smaller cell sizes（about 1-2 μm） owing to their remarkable heterogeneous nucleation effect. Compared to GO reinforced foams, the RGO/PMMA foams own lower cell density and bigger cell size in their microstructure, and their compressive strength is lower even when the reinforcement contents are the same and the foam bulk density is higher. These results indicate that the oxygen-containing groups on GO sheets’ surface are beneficial to adhere CO2 to realize a larger nucleation rate, and their strong interaction with PMMA matrix improves the mechanical property of PMMA foams.
基金supported by the National Natural Science Foundation of China(51902007)。
文摘Water pollution regarding dyes and heavy metal ions is crucial facing the world.How to effectively separate these contaminants from water has been a key issue.Graphene oxide(GO)promises the greenwater world as a long-lasting spotlight adsorbent material and therefore,harnessing GO has been the research hotspot for over a decade.The state of GO as well as its surface functional groups plays an important role in adsorption.And the way of preparation and structural modification matters to the performance of GO.In this review,the significance of the state of existence of stock GO and surface functional groups is explored in terms of preparation,structural modification,and adsorption.Besides,various adsorbates for GO adsorption are also involved,the discussion of which is rarely established elsewhere.
基金funded by the National Natural Science Foundation of China (52100072)the Beijing Natural Science Foundation(8214056)+2 种基金the special fund of Beijing Key Laboratory of Clean Fuels and Efficient Catalytic Emission Reduction Technology,the Strategic Priority Research Program of the Chinese Academy of Sciences(XDA21021101)the National Key Research and Development Program of China (2019YFA0705803)Scientific Research Common Program of Beijing Municipal Commission of Education(KM202010017006)。
文摘FeO;supported on activated carbon(AC) has been shown to be an ideal catalyst for catalytic wet peroxide oxidation(CWPO) due to its high CWPO reaction activity and stability. Although there have been some studies on the mechanism of Fe/AC catalysis in CWPO, the specific contribution of each component(surface oxygen groups and FeOxon AC) inside an Fe/AC catalyst and their corresponding reaction mechanism remain unclear, and the reaction stability of CWPO catalysts has rarely been discussed. Then the optimal CWPO catalyst in our laboratory, 3%Fe/AC, was selected.(1) By removing certain components on the AC through heat treatment, its contribution to the reaction and the corresponding reaction mechanism were investigated. With the aid of temperature-programmed desorption–mass spectrometry(TPD–MS) and the CWPO reaction, the normalized catalytic contributions of components were shown to be: 37.3%(carboxylic groups), 5.3%(anhydride), 19.3%(ether/hydroxyl),-71.4%(carbonyl groups) and 100%(FeOx),respectively. DFT calculation and EPR analysis confirmed that carboxylic groups and Fe_(2)O_(3) are able to activate the H_(2)O_(2) to generate·OH.(2) The catalysts at were characterized at different reaction times(0 h, 450 h, 900 h, 1350 h, and 1800 h) by TPD–MS and M?ssbauer spectroscopy. Results suggested that the number of carboxylic goups gradually increased and the size of paramagnetic Fe_(2)O_(3) particle crystallites gradually increased as the reactions progressed. The occurrence of strong interactions between metal oxides and AC was also confirmed. Due to these effects, the strong stability of 3%Fe/AC was further improved. Therefore, the reasons for the high activity and strong stability of 3%Fe/AC in CWPO were clearly shown. We believe that this work provides an idea of the removal of cresols from wastewater into the introduction to show the potential applications of CWPO.
基金part of the Innovation Program for Undergraduate supported by China University of Mining & Technology,Beijing.
文摘A series of activated carbons（ACs） were prepared using HNO_3,H_2O_2 and steam as activation agents with the aim to introduce functional groups to carbon surface in the ACs preparation process.The effects of concentration of activation agent,activation time on the surface functional groups and redox property of ACs were characterized by Temperature Program Desorption（TPD） and Cyclic Voltammetry（CV）.Results showed that lactone groups of ACs activated by HNO_3 increase with activation time,and the carboxyl groups increase with the concentration of HNO_3.Carbonyl/quinine groups of ACs activated by H_2O_2 increase with the activation time and the concentration of H_2O_2,although the acidic groups decrease with the concentration of H_2O_2.The redox property reflected by CV at 0 and 0.5 V is different with any kinds of oxygen functional groups characterized by TPD,but it is consistent with the SO_2 catalytic oxidization /oxidation properties indicated by TPR.
基金supported by the National Key R&D Program of China(No.2022YFC3203602)the Natural Science Foundation of China(No.52370018)+1 种基金Shaanxi Provincial Youth Innovation Team Project(No.22JP040)Shaanxi Provincial Key Scientific and Technological Innovation Team(No.2023-CX-TD-32).
文摘During the initial impoundment period of a canyon-shaped reservoir,the water body fluctuated violently regarding water level,hydrological condition,and thermal stratification.These variations may alter the structure of phytoplankton community,resulting in algal blooms and seriously threatening the ecological security of the reservoir.It is of great significance to understand the continuous changes of phytoplankton in the initial impoundment period for the protection of reservoir water quality.Therefore,a two-year in-situ monitoring study was conducted on water quality and phytoplankton in a representative canyonshaped reservoir named Sanhekou and the interannual changes of phytoplankton community and its response to environmental changes during the initial impoundment period were discussed at taxonomic versus functional classification levels.The results showed that the total nitrogen and permanganate index levels were relatively high in the first year due to rapid water storage and heavy rainfall input,and the more stable hydrological conditions in the second year promoted the increase of algae density and the transformation of community,and the proportion of cyanobacteria increased significantly.The succession order of phytoplankton in the first year of the initial impoundment periodwas Chlorophyta-Bacillariophyta-Chlorophyta,or J/F/X1-P/MP/W1-A/X1/MP,respectively.And the succession order in the second year was Cyanobacteria/Chlorophyta-Bacillariophyta-Chlorophyta,or L_(M)/G/P-P/A/X1-X1/J/G.Water temperature,relativewater column stability,mixing depth,and pHwere crucial factors affecting phytoplankton community succession.This study revealed the interannual succession law and driving factors of phytoplankton in the initial impoundment period and provided an important reference for the operation management and ecological protection of canyon-shaped reservoirs.
基金This work was supported by the National Natural Science Foundation of China(Nos.22077052,21877052,21907039,22107037)China Postdoctoral Science Foundation(2020M681487,2021M691279)+4 种基金the National Key R&D Program of China(2020YFA0908304)the Natural Science Foundation of Jiangsu Province(BK20180030,BK20190575)the National First-class Discipline Program of Light Industry Technology and Engineering(LITE2018-14)the 111 Project(111-2-06)the Open Project of Key Laboratory of Carbohydrate Chemistry and Biotechnology(Jiangnan University),Ministry of Education(KLCCB-KF202005).
文摘Bacterial surface glycans perform a diverse and important set of biological roles,and have been widely used in the treatment of bacterial infectious diseases.The majority of bacterial surface glycans are decorated with diverse rare functional groups,including amido,acetamidino,carboxamido and pyruvate groups.These functional groups are thought to be important constituents for the biological activities of glycans.Chemical synthesis of glycans bearing these functional groups or their variants is essential for the investigation of structure-activity relationships by a medicinal chemistry approach.To date,a broad choice of synthetic methods is available for targeting the different rare functional groups in bacterial surface glycans.This article reviews the structures of naturally occurring rare functional groups in bacterial surface glycans,and the chemical methods used for installation of these groups.
基金the National Natural Science Foundation of China(No.21978183)。
文摘In this work,a modification method of H_(3)PO_(4)plus H_(2)O_(2)(PHP)was introduced to targetedly form abundant oxygenated functional groups(OFGs)on biochar,and methylene blue(MB)was employed as a model pollutant for adsorption to reflect the modification performance.Results indicated that parent biochars,especially derived from lower temperatures,substantially underwent oxidative modification by PHP,and OFGs were targetedly produced.Correspondingly,approximately 21.5-fold MB adsorption capacity was achieved by PHP-modified biochar comparing with its parent biochar.To evaluate the compatibility of PHP-modification,coefficient of variation(CV)based on MB adsorption capacity by the biochar from various precursors was calculated,in which the CV of PHP-modified biochars was 0.0038 comparing to0.64 of the corresponding parent biochars.These results suggested that the PHP method displayed the excellent feedstock compatibility on biochar modification.The maximum MB adsorption capacity was454.1 mg/g when the H_(3)PO_(4)and H_(2)O_(2)fraction in PHP were 65.2%and 7.0%;the modification was further intensified by promoting temperature and duration.Besides,average 94.5%H_(3)PO_(4)was recovered after 10-batch modification,implying 1.0 kg H_(3)PO_(4)(85%)in PHP can maximally modify 2.37 kg biochar.Overall,this work offered a novel method to tailor biochar towards OFGs-rich surface for efficient adsorption.
基金Project(2012CB722803)supported by the Key Project of National Basic Research and Development Program of ChinaProject(U1202271)supported by the National Natural Science Foundation of ChinaProject(IRT1250)supported by the Program for Innovative Research Team in University of Ministry of Education of China
文摘The industrial silica fume pretreated by nitric acid at 80 °C was re-used in this work. Then, the obtained silica nanoparticles were surface functionalized by silane coupling agents, such as(3-Mercaptopropyl) triethoxysilane(MPTES) and(3-Amincpropyl) trithoxysilane(APTES). Some further modifications were studied by chloroaceetyl choride and 1,8-Diaminoaphalene for amino modified silica. The surface functionalized silica nanoparticles were characterized by Fourier transform infrared(FI-IR) and X-ray photoelectron spectroscopy(XPS). The prepared adsorbent of surface functionalized silica nanoparticles with differential function groups were investigated in the selective adsorption about Pb2+, Cu2+, Hg2+, Cd2+ and Zn2+ions in aqueous solutions. The results show that the(3-Mercaptopropyl) triethoxysilane functionalized silica nanoparticles(SiO2-MPTES) play an important role in the selective adsorption of Cu2+ and Hg2+, the(3-Amincpropyl) trithoxysilane(APTES) functionalized silica nanoparticles(SiO2-APTES) exhibited maximum removal efficiency towards Pb2+ and Hg2+, the 1,8-Diaminoaphalene functionalized silica nanoparticles was excellent for removal of Hg2+ at room temperature, respectively.
基金supported by the Innovative Research Group Project of the National Natural Science Foundation of China(T2121004)Key Programme(52235007)National Outstanding Youth Foundation of China(52325504).
文摘Hydrogel scaffolds have numerous potential applications in the tissue engineering field.However,tough hydrogel scaffolds implanted in vivo are seldom reported because it is difficult to balance biocompatibility and high mechanical properties.Inspired by Chinese ramen,we propose a universal fabricating method(printing-P,training-T,cross-linking-C,PTC&PCT)for tough hydrogel scaffolds to fill this gap.First,3D printing fabricates a hydrogel scaffold with desired structures(P).Then,the scaffold could have extraordinarily high mechanical properties and functional surface structure by cycle mechanical training with salting-out assistance(T).Finally,the training results are fixed by photo-cross-linking processing(C).The tough gelatin hydrogel scaffolds exhibit excellent tensile strength of 6.66 MPa(622-fold untreated)and have excellent biocompatibility.Furthermore,this scaffold possesses functional surface structures from nanometer to micron to millimeter,which can efficiently induce directional cell growth.Interestingly,this strategy can produce bionic human tissue with mechanical properties of 10 kPa-10 MPa by changing the type of salt,and many hydrogels,such as gelatin and silk,could be improved with PTC or PCT strategies.Animal experiments show that this scaffold can effectively promote the new generation of muscle fibers,blood vessels,and nerves within 4 weeks,prompting the rapid regeneration of large-volume muscle loss injuries.
基金funding of the National Key Research and Development Plan(Grant 2017YFB0306600)the Project of SINOPEC(NO.117006).
文摘To prepare a highly efficient NiMo/Al_(2)O_(3) hydrodesulfurization catalyst,the combined effects of specific organic functional groups and alumina surface characteristics were investigated.First,the correlation between the surface characteristics of four different alumina and the existing Mo species states was established.It was found that the Mo equilibrium adsorption capacity can be used as a specific descriptor to quantitatively evaluate the changes in surface characteristics of different alumina.A lower Mo equilibrium adsorption capacity for alumina means weaker metal-support interaction and the loaded Mo species are easier to transform into MoS2.However,the Mo-O-Al bonds still exist at the metal-support interface.The introduction of cationic surfactant hecadecyl trimethyl ammonium bromide(CTAB)can further improve Mo species dispersion through electrostatic attraction with Mo anions and interaction of its alkyl chain with the alumina surface;meanwhile,the introduction of ethylenediamine tetraacetic acid(EDTA)can complex with Ni ions to enhance the Ni-promoting effect on Mo.Therefore,the NiMo catalyst designed using alumina with lower Mo equilibrium adsorption capacity and the simultaneous addition of EDTA and CTAB exhibits the highest hydrodesulfurization activity for 4,6-dimethyl dibenzothiophene because of its proper metal-support interaction and more well-dispersed Ni-Mo-S active phases.
基金supported by the National Science Foundation of China(No.21606191)the Natural Science Foundation of Shandong Province(No.ZR2020ME024).
文摘As a new electrochemical technology,capacitive deionization(CDI)has been increasingly applied in environmental water treatment and seawater desalination.In this study,functional groups modified porous hollow carbon(HC)were synthesized as CDI electrode material for removing Na^(+)and Cl^(−)in salty water.Results showed that the average diameter of HC was approximately 180 nm,and the infrared spectrum showed that its surface was successfully modified with sulfonic and amino groups,respectively.The sulfonic acid functionalized HC(HC-S)showed better electrochemical and desalting performance than the amino-functionalized HC(HC–N),with a maximum Faradic capacity of 287.4 F/g and an adsorptive capacity of 112.97 mg/g for NaCl.Additionally,92.63%capacity retention after 100 adsorption/desorption cycles demonstrates the excellent stability of HC-S.The main findings prove that HC-S is viable as an electrodematerial for desalination by high-performance CDI applications.
基金financially supported by the Shenzhen Science and Technology Project(Project Nos.JCYJ20220818102201003,JCYJ20220818100001002)the Shenzhen Sustainable Development Special Project(Project No.KCXFZ20230731094500001)+1 种基金the National Natural Science Foundation of China(Project Nos.51975597,52175446)the Natural Science Foundation of Guangdong Province(Project No.2022B1515020011)。
文摘Magnetically responsive microstructured functional surface(MRMFS),capable of dynamically and reversibly switching the surface topography under magnetic actuation,provides a wireless,noninvasive,and instantaneous way to accurately control the microscale engineered surface.In the last decade,many studies have been conducted to design and optimize MRMFSs for diverse applications,and significant progress has been accomplished.This review comprehensively presents recent advancements and the potential prospects in MRMFSs.We first classify MRMFSs into one-dimensional linear array MRMFSs,two-dimensional planar array MRMFSs,and dynamic self-assembly MRMFSs based on their morphology.Subsequently,an overview of three deformation mechanisms,including magnetically actuated bending deformation,magnetically driven rotational deformation,and magnetically induced self-assembly deformation,are provided.Four main fabrication strategies employed to create MRMFSs are summarized,including replica molding,magnetization-induced self-assembly,laser cutting,and ferrofluid-infused method.Furthermore,the applications of MRMFS in droplet manipulation,solid transport,information encryption,light manipulation,triboelectric nanogenerators,and soft robotics are presented.Finally,the challenges that limit the practical applications of MRMFSs are discussed,and the future development of MRMFSs is proposed.
文摘Rayon-based carbon fibers were anodically oxidized in the presence of a variety of electrolytes. The functional groups produced on carbon fiber surface were characterized by Fourier Transform Infrared Spectroscopy (FTIR). Both K Br pellet spectra and ATR difference spectra indicate that carboxyl and phenolic and carbonyl groups were produced. The acidic groups, carboxyl and phenol, were measured by potentiometrie titration with standard solutions of acid and alkali. The results show that the amount of acidic groups is related to the electrolyte used.
基金Supported by the National Natural Science Foundation of China(42172148,42172142)。
文摘Taking the Lower Silurian Longmaxi Formation shale in the Sichuan Basin as an example,this study employs atomic force microscopy-based infrared(AFM-IR)spectroscopy to analyze the submicron-scale molecular functional groups of different types and occurrences of organic matter.Combined with the quantitative evaluation of pore development via scanning electron microscopy(SEM),the response of organic pore formation and evolution mechanisms to chemical composition and structural evolution of organic matter in overmature marine shale is investigated.The results indicate that the AFM-IR spectra of graptolite periderms and pyrobitumen in shale are dominated by the stretching vibrations of conjugated C=C bonds in aromatic compounds at approximately 1600 cm-1,with weak absorption peaks near 1375,1450 and 1720 cm-1,corresponding to aliphatic chains and carbonyl/carboxyl functional groups.Overall,the AFM-IR structural indices(A and C factors)of organic matter show a strong correlation with visible porosity in shales of equivalent maturity.Lower A and C factor values correlate with enhanced development of organic pores,which is associated with the detachment of more aliphatic chains and oxygen-containing functional groups during thermal evolution.Pyrobitumen-clay mineral composites generally exhibit superior pore development,likely attributable to clay mineral dehydration participating in hydrocarbon generation reactions that promote the removal of more functional groups.Additionally,hydrocarbon generation within organic-clay composites during high-over mature stages may induce volumetric expansion,resulting in microfracturing and hydrocarbon expulsion.The associated higher hydrocarbon expulsion rates promote the formation of larger pores and fracture-shaped pores along the flake-shaped clay minerals.This study highlights that the research of submicron-scale molecular functional groups provides a deeper understanding of organic matter evolution and pores development mechanisms in overmature shales,thereby offering critical theoretical parameters for reservoir evaluation in shale oil and gas exploration.
文摘Biomass-derived carbon materials are favored for their abundance and sustainability,and ease of preparation and modification.By surface activation and modification they can have a good electrical conductivity,excellent catalytic activity,a remarkable adsorption capacity,and different interfacial physicochemical functionalities.Surface-modified biochars have found wide applications in energy storage,environmental remediation,and catalysis.However,achieving precise and controllable modification of their active sites remains a challenge.Recent advances and future prospects for controlling their surface morphology,defect engineering,and surface coating strategies,with particular attention to their means of fabrication,are reviewed.
