Low-concentration coal mine methane(LC-CMM),which is predominantly composed of methane,serves as a clean and low-carbon energy resource with significant potential for utilization.Utilizing LC-CMM as fuel for solid oxi...Low-concentration coal mine methane(LC-CMM),which is predominantly composed of methane,serves as a clean and low-carbon energy resource with significant potential for utilization.Utilizing LC-CMM as fuel for solid oxide fuel cells(SOFCs)represents an efficient and promising strategy for its effective utilization.However,direct application in Ni-based anodes induces carbon deposition,which severely degrades cell performance.Herein,a medium-entropy oxide Sr_(2)FeNi_(0.1)Cr_(0.3)Mn_(0.3)Mo_(0.3)O_(6−δ)(SFNCMM)was developed as an anode internal reforming catalyst.Following reduction treatment,FeNi_(3) nano-alloy particles precipitate on the surface of the material,thereby significantly enhancing its catalytic activity for LC-CMM reforming process.The catalyst achieved a methane conversion rate of 53.3%,demonstrating excellent catalytic performance.Electrochemical evaluations revealed that SFNCMM-Gd_(0.1)Ce_(0.9)O_(2−δ)(GDC)with a weight ratio of 7:3 exhibited superior electrochemical performance when employed as the anodic catalytic layer.With H_(2) and LC-CMM as fuels,the single cell achieved maximum power densities of 1467.32 and 1116.97 mW·cm^(−2) at 800℃,respectively,with corresponding polarization impedances of 0.17 and 1.35Ω·cm^(2).Furthermore,the single cell maintained stable operation for over 100 h under LC-CMM fueling without significant carbon deposition,confirming its robust resistance to carbon formation.These results underscore the potential of medium-entropy oxides as highly effective catalytic layers for mitigating carbon deposition in SOFCs.展开更多
This research reports a novel heterogeneous Fenton-like catalyst which could freely move through the model sediments and easily seize the pollutants in addition to efficiently catalyze H2O2,well suitable for soil and ...This research reports a novel heterogeneous Fenton-like catalyst which could freely move through the model sediments and easily seize the pollutants in addition to efficiently catalyze H2O2,well suitable for soil and groundwater remediation.Herein,submicron y-Fe2O3/C spheres were synthesized through a facile one-step aerosol-based process.In a series of column tests,these spheres exhibit better transport ability due to their optimal size,conforming to the prediction by the Tufenkji-Elimelech filtration theo ry.Meanwhile,y-Fe2O3/C spheres could act as a strong adsorbent for organic pollutants owing to the presence of carbon,thereby providing a driving force to gather contaminants into their vicinity and facilitating the reaction.In addition,immobilization of y-Fe2O3 nanoparticles into carbon spheres protects iron oxides from aggregation,and thus retains the number of active sites for catalytic decomposition of H2O2.Hence,the system containing the as-prepared y-Fe2O3/C spheres and H2O2 shows the high removal efficiency and degradation efficiency in the remediation of recalcitrant organic contaminants such as methylene blue and sulfamethoxazole.展开更多
The aromatic nature of lignin makes it a potential renewable source of chemicals and other valuable products.Isolation of lignin from lignocellulosic biomass using organic solvents enables the production of high-purit...The aromatic nature of lignin makes it a potential renewable source of chemicals and other valuable products.Isolation of lignin from lignocellulosic biomass using organic solvents enables the production of high-purity lignin.The use of formic acid in the organosolv pulping and fractionation process has been widely studied.Characterization of lignin is necessary to achieve valueadded applications of lignin.To simplify the isolation of formic acid-treated lignin,herein,milled wheat straw lignin(MWSL) was employed as an archetype for characterization of the structural changes of lignin during formic acid treatment.The results showed that the MWSL was GSH-type(comprising p-hydroxyphenyl(H),guaiacyl(G),and syringyl(S) monolignols) and underwent structural changes during formic acid treatment.Lignin was esterified during the formic acid treatment.The content of alkyl hydroxyl groups in lignin decreased upon formic acid treatment,corresponding to an increase of the number of double bond equivalents(DBE).Lignin units with active reaction sites were liable to slight condensation,which resulted in a moderate increase of the molecular weight.The molecular weight distribution of formic acid-treated MWSL(FMWSL) was wider than that of the MWSL,although the molecular weight of both species did not differ significantly.The β-O-4 linkage in lignin was partially cleaved during formic acid treatment,resulting in the production of new phenolic structures.This improved the solubility of lignin in the cooking liquor and its reactivity for downstream applications.展开更多
With the emergence of Y-series small molecule acceptors,polymerizing the small molecule acceptors with aromatic linker units has attracted significant research attention,which has greatly advanced the photovoltaic per...With the emergence of Y-series small molecule acceptors,polymerizing the small molecule acceptors with aromatic linker units has attracted significant research attention,which has greatly advanced the photovoltaic performance of all-polymer solar cells.Despite the rapid increase in efficiency,the unique characteristics(e.g.,mechanical stretchability and flexibility)of all-polymer systems were still not thoroughly explored.In this work,we demonstrate an effective approach to simultaneously improve device performance,stability,and mechanical robustness of all-polymer solar cells by properly suppressing the aggregation and crystallization behaviors of polymerized Y-series acceptors.Strikingly,when introducing 50 wt%PYF-IT(a fluorinated version of PY-IT)into the well-known PM6:PY-IT system,the all-polymer devices delivered an impressive photovoltaic efficiency of 16.6%,significantly higher than that of the control binary cell(15.0%).Compared with the two binary systems,the optimal ternary blend exhibits more efficient charge separation and balanced charge transport accompanying with less recombination.Moreover,a high-performance 1.0 cm^(2)large-area device of 15%efficiency was demonstrated for the optimized ternary all-polymer blend,which offered a desirable PCE of 14.5%on flexible substrates and improved mechanical flexibility after bending 1000 cycles.Notably,these are among the best results for 1.0 cm^(2)all-polymer OPVs thus far.This work also heralds a bright future of all-polymer systems for flexible wearable energy-harvesting applications.展开更多
With the rapid increase in photoelectric conversion efficiency of organic photovoltaics(OPVs),prolonging the operational lifetime of devices becomes one of the critical prerequisites for commercial applications.Guided...With the rapid increase in photoelectric conversion efficiency of organic photovoltaics(OPVs),prolonging the operational lifetime of devices becomes one of the critical prerequisites for commercial applications.Guided by the theoretical calculations of molecular stacking and miscibility,we proposed an effective approach to simultaneously improve device performance and thermal stability of high-efficiency OPVs by refining the aggregation of Y-series acceptors.The key to this approach is deliberately designing an asymmetric Y-series acceptor,named Y6-CNO,which acts as a third component regulator to finely tune the degree of acceptor aggregation and crystallization in the benchmark PM6:Y6-BO system.Strikingly,a champion photovoltaic efficiency of 18.0%was achieved by introducing 15 wt%Y6-CNO into the PM6:Y6-BO system,significantly higher than the control binary cell(16.7%).Moreover,annealing at 100°C for over 1,200 h does not markedly affect the photovoltaic performance of the optimal ternary devices,maintaining above 95%of the initial performance and exhibiting an exceptionally high T_(80)lifetime of 9,000 h under continuous thermal annealing.By contrast,binary devices suffer from excessive crystallization of acceptors with long-term annealing.Additionally,mixing thermodynamics combined with morphological characterizations were employed to elucidate the microstructure-thermal stability relationships.The ternary OPVs consisting of symmetric and asymmetric homologous acceptors form better charge transport channels and can effectively suppress excessive aggregation of acceptors under long-term annealing.This work demonstrates the effectiveness of refining acceptor aggregation via molecular design for highly efficient and stable nonfullerene-based OPVs.展开更多
Materials exhibiting time-dependent phosphorescence color(TDPC)are attractive,but generally suffer from complex preparation processes and low-color contrast.Herein,molecular aggregation regulation of 1-pyrenecarboxyli...Materials exhibiting time-dependent phosphorescence color(TDPC)are attractive,but generally suffer from complex preparation processes and low-color contrast.Herein,molecular aggregation regulation of 1-pyrenecarboxylic acid(PyC)in the konjac glucomannan(KGM)matrix is proposed to realize high-contrast TDPC.The steric hindrance of KGM enables isolated state,carboxyl dimer,andπ-stacking-induced multimers of PyC with different phosphorescence wavelengths and lifetimes to coexist,leading to a typical TDPC evolution from red to blue-green.The TDPC shows remarkable phosphorescence wavelength shift up to 182 nm and phosphorescence lifetime up to 788.43 ms,readily recognized by the naked eye.In addition,KGM,an edible natural polysaccharide,displays decent rheological properties suitable for screen printing,film casting,and 3D printing,making PyC-KGM an eco-friendly tool for multi-dimensional information security applications.The work provides a simple yet efficient method for high-contrast TDPC materials and affords a promising material for high-level dynamic information encryption and anti-counterfeiting.展开更多
基金supported by the National Key R&D Program of China(No.2024YFB4007501)the Natural Science Foundation of Jiangsu Province(No.BK20240109)the project of Jiangsu Key Laboratory for Clean Utilization of Carbon Resources(No.BM2024007).
文摘Low-concentration coal mine methane(LC-CMM),which is predominantly composed of methane,serves as a clean and low-carbon energy resource with significant potential for utilization.Utilizing LC-CMM as fuel for solid oxide fuel cells(SOFCs)represents an efficient and promising strategy for its effective utilization.However,direct application in Ni-based anodes induces carbon deposition,which severely degrades cell performance.Herein,a medium-entropy oxide Sr_(2)FeNi_(0.1)Cr_(0.3)Mn_(0.3)Mo_(0.3)O_(6−δ)(SFNCMM)was developed as an anode internal reforming catalyst.Following reduction treatment,FeNi_(3) nano-alloy particles precipitate on the surface of the material,thereby significantly enhancing its catalytic activity for LC-CMM reforming process.The catalyst achieved a methane conversion rate of 53.3%,demonstrating excellent catalytic performance.Electrochemical evaluations revealed that SFNCMM-Gd_(0.1)Ce_(0.9)O_(2−δ)(GDC)with a weight ratio of 7:3 exhibited superior electrochemical performance when employed as the anodic catalytic layer.With H_(2) and LC-CMM as fuels,the single cell achieved maximum power densities of 1467.32 and 1116.97 mW·cm^(−2) at 800℃,respectively,with corresponding polarization impedances of 0.17 and 1.35Ω·cm^(2).Furthermore,the single cell maintained stable operation for over 100 h under LC-CMM fueling without significant carbon deposition,confirming its robust resistance to carbon formation.These results underscore the potential of medium-entropy oxides as highly effective catalytic layers for mitigating carbon deposition in SOFCs.
基金supported by the National Natural Science Foundation of China(NSFC,Nos.21876022,31400840)the Fundamental Research Funds for the Central Universities(No.DUT16ZD226)PetroChina Innovation Foundation(No.2017D5007-0609)。
文摘This research reports a novel heterogeneous Fenton-like catalyst which could freely move through the model sediments and easily seize the pollutants in addition to efficiently catalyze H2O2,well suitable for soil and groundwater remediation.Herein,submicron y-Fe2O3/C spheres were synthesized through a facile one-step aerosol-based process.In a series of column tests,these spheres exhibit better transport ability due to their optimal size,conforming to the prediction by the Tufenkji-Elimelech filtration theo ry.Meanwhile,y-Fe2O3/C spheres could act as a strong adsorbent for organic pollutants owing to the presence of carbon,thereby providing a driving force to gather contaminants into their vicinity and facilitating the reaction.In addition,immobilization of y-Fe2O3 nanoparticles into carbon spheres protects iron oxides from aggregation,and thus retains the number of active sites for catalytic decomposition of H2O2.Hence,the system containing the as-prepared y-Fe2O3/C spheres and H2O2 shows the high removal efficiency and degradation efficiency in the remediation of recalcitrant organic contaminants such as methylene blue and sulfamethoxazole.
文摘The aromatic nature of lignin makes it a potential renewable source of chemicals and other valuable products.Isolation of lignin from lignocellulosic biomass using organic solvents enables the production of high-purity lignin.The use of formic acid in the organosolv pulping and fractionation process has been widely studied.Characterization of lignin is necessary to achieve valueadded applications of lignin.To simplify the isolation of formic acid-treated lignin,herein,milled wheat straw lignin(MWSL) was employed as an archetype for characterization of the structural changes of lignin during formic acid treatment.The results showed that the MWSL was GSH-type(comprising p-hydroxyphenyl(H),guaiacyl(G),and syringyl(S) monolignols) and underwent structural changes during formic acid treatment.Lignin was esterified during the formic acid treatment.The content of alkyl hydroxyl groups in lignin decreased upon formic acid treatment,corresponding to an increase of the number of double bond equivalents(DBE).Lignin units with active reaction sites were liable to slight condensation,which resulted in a moderate increase of the molecular weight.The molecular weight distribution of formic acid-treated MWSL(FMWSL) was wider than that of the MWSL,although the molecular weight of both species did not differ significantly.The β-O-4 linkage in lignin was partially cleaved during formic acid treatment,resulting in the production of new phenolic structures.This improved the solubility of lignin in the cooking liquor and its reactivity for downstream applications.
基金This research was made possible thanks to the financial support of the National Natural Science Foundation of China(Nos.52073207 and 52121002)the Fundamental Research Funds for the Central Universities.L.Ye also appreciates the Peiyang Scholar Program of Tianjin University for support。
文摘With the emergence of Y-series small molecule acceptors,polymerizing the small molecule acceptors with aromatic linker units has attracted significant research attention,which has greatly advanced the photovoltaic performance of all-polymer solar cells.Despite the rapid increase in efficiency,the unique characteristics(e.g.,mechanical stretchability and flexibility)of all-polymer systems were still not thoroughly explored.In this work,we demonstrate an effective approach to simultaneously improve device performance,stability,and mechanical robustness of all-polymer solar cells by properly suppressing the aggregation and crystallization behaviors of polymerized Y-series acceptors.Strikingly,when introducing 50 wt%PYF-IT(a fluorinated version of PY-IT)into the well-known PM6:PY-IT system,the all-polymer devices delivered an impressive photovoltaic efficiency of 16.6%,significantly higher than that of the control binary cell(15.0%).Compared with the two binary systems,the optimal ternary blend exhibits more efficient charge separation and balanced charge transport accompanying with less recombination.Moreover,a high-performance 1.0 cm^(2)large-area device of 15%efficiency was demonstrated for the optimized ternary all-polymer blend,which offered a desirable PCE of 14.5%on flexible substrates and improved mechanical flexibility after bending 1000 cycles.Notably,these are among the best results for 1.0 cm^(2)all-polymer OPVs thus far.This work also heralds a bright future of all-polymer systems for flexible wearable energy-harvesting applications.
基金supported by the National Natural Science Foundation of China(52073207,52121002)the Fundamental Research Funds for the Central Universities+1 种基金the Peiyang Scholar Program of Tianjin University for supportthe Haihe Laboratory of Sustainable Chemical Transformations for financial support。
文摘With the rapid increase in photoelectric conversion efficiency of organic photovoltaics(OPVs),prolonging the operational lifetime of devices becomes one of the critical prerequisites for commercial applications.Guided by the theoretical calculations of molecular stacking and miscibility,we proposed an effective approach to simultaneously improve device performance and thermal stability of high-efficiency OPVs by refining the aggregation of Y-series acceptors.The key to this approach is deliberately designing an asymmetric Y-series acceptor,named Y6-CNO,which acts as a third component regulator to finely tune the degree of acceptor aggregation and crystallization in the benchmark PM6:Y6-BO system.Strikingly,a champion photovoltaic efficiency of 18.0%was achieved by introducing 15 wt%Y6-CNO into the PM6:Y6-BO system,significantly higher than the control binary cell(16.7%).Moreover,annealing at 100°C for over 1,200 h does not markedly affect the photovoltaic performance of the optimal ternary devices,maintaining above 95%of the initial performance and exhibiting an exceptionally high T_(80)lifetime of 9,000 h under continuous thermal annealing.By contrast,binary devices suffer from excessive crystallization of acceptors with long-term annealing.Additionally,mixing thermodynamics combined with morphological characterizations were employed to elucidate the microstructure-thermal stability relationships.The ternary OPVs consisting of symmetric and asymmetric homologous acceptors form better charge transport channels and can effectively suppress excessive aggregation of acceptors under long-term annealing.This work demonstrates the effectiveness of refining acceptor aggregation via molecular design for highly efficient and stable nonfullerene-based OPVs.
基金supported by the National Science Fund for Distinguished Young Scholars of China(32225034)the National Natural Science Foundation of China(22308028)+1 种基金the Fundamental Research Funds for the Central Universities(JCYJ202501)the Young Elite Scientists Sponsorship Program by CAST(YESS20240208).
文摘Materials exhibiting time-dependent phosphorescence color(TDPC)are attractive,but generally suffer from complex preparation processes and low-color contrast.Herein,molecular aggregation regulation of 1-pyrenecarboxylic acid(PyC)in the konjac glucomannan(KGM)matrix is proposed to realize high-contrast TDPC.The steric hindrance of KGM enables isolated state,carboxyl dimer,andπ-stacking-induced multimers of PyC with different phosphorescence wavelengths and lifetimes to coexist,leading to a typical TDPC evolution from red to blue-green.The TDPC shows remarkable phosphorescence wavelength shift up to 182 nm and phosphorescence lifetime up to 788.43 ms,readily recognized by the naked eye.In addition,KGM,an edible natural polysaccharide,displays decent rheological properties suitable for screen printing,film casting,and 3D printing,making PyC-KGM an eco-friendly tool for multi-dimensional information security applications.The work provides a simple yet efficient method for high-contrast TDPC materials and affords a promising material for high-level dynamic information encryption and anti-counterfeiting.
