The integration of selective oxidation of renewable biomass and its derivatives with hydrogen(H_(2))pro-duction holds significant potential for simultaneously yielding value-added chemicals and“green H_(2)”,contribu...The integration of selective oxidation of renewable biomass and its derivatives with hydrogen(H_(2))pro-duction holds significant potential for simultaneously yielding value-added chemicals and“green H_(2)”,contributing to addressing sustainability challenges.The S-scheme charge transfer mechanism enhances charge separation by maintaining strong redox potentials at both ends,facilitating both oxidation and reduction reactions.Herein,we synthesize a visible-light-responsive oxygen vacancy-rich In_(2)O_(3-x)/tubular carbon nitride(IO_(OV)/TCN)S-scheme heterojunction photocatalyst via electrostatic adherence for selec-tive 5-hydroxymethylfurfural(HMF)oxidation to 2,5-diformylfuran(DFF)and 2,5-furandicarboxylic acid(FDCA),alongside H_(2)production.Under anaerobic conditions and visible-light irradiation,the optimal IOOV/TCN-10 catalyst achieves an HMF conversion of 94.8%with a selectivity of 53.6%for DFF and FDCA,and a H_(2)yield of 754.05μmol g^(−1)in 3 h.The significantly improved photocatalytic activity results from enhanced visible-light absorption,reduced carrier recombination,and abundant catalytic active sites due to the synergistic effect of surface oxygen vacancies,the hollow nanotube-based architecture,and the S-scheme charge transfer mechanism.This work highlights the great potentials of S-scheme heterojunctions in biomass conversion for sustainable energy use and chemical production.展开更多
The problem of water and sulfur poisoning in flue gas atmosphere remains a significant obstacle for low-temperature deNO_(x) catalysts.This study investigated the sulfation mechanism of the CoMn_(2)O_(4)/CeTiO_(x)(CMC...The problem of water and sulfur poisoning in flue gas atmosphere remains a significant obstacle for low-temperature deNO_(x) catalysts.This study investigated the sulfation mechanism of the CoMn_(2)O_(4)/CeTiO_(x)(CMCT)catalyst during the selective catalytic reduction of NO_(x) with NH3 under conditions containing H2O and SO_(2) at 150℃.Employing a comprehensive suite of time-resolved analysis and characterization techniques,the evolution of sulfate species was systematically categorized into three stages:initial rapid surface sulfate accumulation,the transformation of surface sulfates to bulk metal sulfates,and partial sulfates decomposition after the removal of H2O and SO_(2).These findings indicate that bulk metal sulfates irreversibly deactivate the catalyst by distorting active component lattices and consuming oxygen vacancies,whereas surface sulfates(including ammonium sulfates and surface-coordinated metal sulfates)cause reversible performance loss through decomposition.Furthermore,the competitive adsorption of H2O and SO_(2) significantly influences the catalytic efficiency,with H2O suppressing SO_(2) adsorption while simultaneously enhancing the formation of Brönsted acid sites.This research underscores the critical role of sulfate dynamics on catalyst performance,revealing the enhanced SO_(2) resistance of the Eley-Rideal mechanism facilitated by the Ce-Ti support relative to the Langmuir-Hinshelwood pathway.Collectively,the study unravels the complex interplay of sulfate dynamics influencing catalyst performance and provides potential approaches to mitigate deactivation in demanding atmospheric conditions.展开更多
The removal of four dissolved organic matter(DOM) fractions, non-acid hydrophobics,hydrophobic acids, hydrophilics and transphilics, was achieved by coagulation-UV/H_2O_2 oxidation in post-pharmaceutical wastewater(Ph...The removal of four dissolved organic matter(DOM) fractions, non-acid hydrophobics,hydrophobic acids, hydrophilics and transphilics, was achieved by coagulation-UV/H_2O_2 oxidation in post-pharmaceutical wastewater(PhW W). Coagulation with Polyferric chloride(PFC), Polymeric ferric sulfate(PFS) and Polymeric aluminum ferric chloride(PAFC) was studied separately to evaluate the effects of the initial pH and coagulant dosage. The coagulation-UV/H_2O_2 oxidation method resulted in much higher reduction rates for dissolved organic carbon(DOC)(by 75%) and UV_(254)(by 92%) than coagulation or UV/H_2O_2 oxidation alone. The proportion of non-acid hydrophobics, hydrophobic acids, transphilics and hydrophilics removed by coagulation was 54%, 49%, 27% and 12 %, while the combined treatment removed 92%, 87%,70% and 39%, respectively. Parallel factor analysis(PARAFAC) of fluorescence measurements revealed that the humic-like fluorescent component C4 showed the highest removal(by 44%)during the coagulation stage. After coagulation-UV/H_2O_2 treatment, the humic-like fluorescent component C3 had the highest removal(by 72%), whereas xenobiotic organic fluorescent components C1 and C4 remained recalcitrant to decomposition. Significant correlations(R2> 0.8)between C1 and the hydrophobic acids and non-acid hydrophobics suggested the possibility of using fluorescence spectroscopy as an effective tool to assess variations in DOM fraction treatment efficacy in coagulation-UV/H_2O_2 systems. After the combined treatment, toxic inhibition of cellular activity by post PhW W decreased from 88% to 47% and biodegradability increased from 0.1 to 0.52.展开更多
制备了负载在Na Y分子筛上的Fe Cu Mn Y复合催化剂,并对其在非均相UV Fe Cu Mn Y H2O2体系中催化氧化4BS染料废水进行了研究.结果表明,非均相UV Fe Cu Mn Y H2O2体系对4BS染料废水的处理具有很高的效率.在基准条件下,反应时间为20min时...制备了负载在Na Y分子筛上的Fe Cu Mn Y复合催化剂,并对其在非均相UV Fe Cu Mn Y H2O2体系中催化氧化4BS染料废水进行了研究.结果表明,非均相UV Fe Cu Mn Y H2O2体系对4BS染料废水的处理具有很高的效率.在基准条件下,反应时间为20min时,废水中4BS的去除率达到了93 7%.与均相UV Fenton体系不同,非均相UV Fe Cu Mn Y H2O2体系在碱性条件下(pH=10 5)仍可高效去除CODCr.动力学研究得到催化氧化4BS废水的模型方程,该模型可以为非均相UV Fe Cu Mn Y H2O2体系处理高色度的实际染料废水提供指导.展开更多
The degradation of formaldehyde gas was studied using UV/TiO2/O3 process under the condition of continuous flow mode. The effects of humidity, initial formaldehyde concentration, residence time and ozone adding amount...The degradation of formaldehyde gas was studied using UV/TiO2/O3 process under the condition of continuous flow mode. The effects of humidity, initial formaldehyde concentration, residence time and ozone adding amount on degradation of formaldehyde gas were investigated. The experimental results indicated that the combination of ozonation with photocatalytic oxidation on the degradation of formaldehyde showed a synergetic action, e.g,, it could considerably increase decomposing of formaldehyde. The degradation efficiency of formaldehyde was between 73.6% and 79.4% while the initial concentration in the range of 1.84--24 mg/m^3 by O3/TiO2flJV process. The optimal humidity was about 50% in UV/TiO2/O3 processs and degradation of formaldehyde increases from 39.0% to 94.1% when the ozone content increased from 0 to 141 mg/m^3. Furthermore, the kinetics of formaldehyde degradation reaction could be described by Langmuir-Hinshelwood model. The rate constant k of 46.72 mg/（m^3.min） and Langmuir adsorption coefficient K of 0.0268 m^3/mg were obtained.展开更多
In order to purify oil recovery wastewater from polymer flooding （ORWPF） in tertiary oil recovery in oil fields, advanced treatment of UV/H2O2/O3 and fine filtration were investigated. The experimental results showe...In order to purify oil recovery wastewater from polymer flooding （ORWPF） in tertiary oil recovery in oil fields, advanced treatment of UV/H2O2/O3 and fine filtration were investigated. The experimental results showed that polyacrylamide and oil remaining in ORWPF after the conventional treatment process could be effectively removed by UV/H2O2/O3 process. Fine filtration gave a high performance in eliminating suspended solids. The treated ORWPF can meet the quality requirement of the wastewater-bearing polymer injection in oilfield and be safely re-injected into oil reservoirs for oil recovery.展开更多
基金financially supported by the Natural Science Foundation of China(Nos.21972058,22102064,and 22302080)Anhui Key Laboratory of Nanomaterials and Nanotechnology,the Major Science and Technology Projects in Anhui Province(No.202305a12020006).
文摘The integration of selective oxidation of renewable biomass and its derivatives with hydrogen(H_(2))pro-duction holds significant potential for simultaneously yielding value-added chemicals and“green H_(2)”,contributing to addressing sustainability challenges.The S-scheme charge transfer mechanism enhances charge separation by maintaining strong redox potentials at both ends,facilitating both oxidation and reduction reactions.Herein,we synthesize a visible-light-responsive oxygen vacancy-rich In_(2)O_(3-x)/tubular carbon nitride(IO_(OV)/TCN)S-scheme heterojunction photocatalyst via electrostatic adherence for selec-tive 5-hydroxymethylfurfural(HMF)oxidation to 2,5-diformylfuran(DFF)and 2,5-furandicarboxylic acid(FDCA),alongside H_(2)production.Under anaerobic conditions and visible-light irradiation,the optimal IOOV/TCN-10 catalyst achieves an HMF conversion of 94.8%with a selectivity of 53.6%for DFF and FDCA,and a H_(2)yield of 754.05μmol g^(−1)in 3 h.The significantly improved photocatalytic activity results from enhanced visible-light absorption,reduced carrier recombination,and abundant catalytic active sites due to the synergistic effect of surface oxygen vacancies,the hollow nanotube-based architecture,and the S-scheme charge transfer mechanism.This work highlights the great potentials of S-scheme heterojunctions in biomass conversion for sustainable energy use and chemical production.
文摘The problem of water and sulfur poisoning in flue gas atmosphere remains a significant obstacle for low-temperature deNO_(x) catalysts.This study investigated the sulfation mechanism of the CoMn_(2)O_(4)/CeTiO_(x)(CMCT)catalyst during the selective catalytic reduction of NO_(x) with NH3 under conditions containing H2O and SO_(2) at 150℃.Employing a comprehensive suite of time-resolved analysis and characterization techniques,the evolution of sulfate species was systematically categorized into three stages:initial rapid surface sulfate accumulation,the transformation of surface sulfates to bulk metal sulfates,and partial sulfates decomposition after the removal of H2O and SO_(2).These findings indicate that bulk metal sulfates irreversibly deactivate the catalyst by distorting active component lattices and consuming oxygen vacancies,whereas surface sulfates(including ammonium sulfates and surface-coordinated metal sulfates)cause reversible performance loss through decomposition.Furthermore,the competitive adsorption of H2O and SO_(2) significantly influences the catalytic efficiency,with H2O suppressing SO_(2) adsorption while simultaneously enhancing the formation of Brönsted acid sites.This research underscores the critical role of sulfate dynamics on catalyst performance,revealing the enhanced SO_(2) resistance of the Eley-Rideal mechanism facilitated by the Ce-Ti support relative to the Langmuir-Hinshelwood pathway.Collectively,the study unravels the complex interplay of sulfate dynamics influencing catalyst performance and provides potential approaches to mitigate deactivation in demanding atmospheric conditions.
基金supported by the National Key Scientific and Technological Project for Water Pollution Control and Management (Nos.2012ZX07202-005,2012ZX07202-002,2014 ZX07216001-2)
文摘The removal of four dissolved organic matter(DOM) fractions, non-acid hydrophobics,hydrophobic acids, hydrophilics and transphilics, was achieved by coagulation-UV/H_2O_2 oxidation in post-pharmaceutical wastewater(PhW W). Coagulation with Polyferric chloride(PFC), Polymeric ferric sulfate(PFS) and Polymeric aluminum ferric chloride(PAFC) was studied separately to evaluate the effects of the initial pH and coagulant dosage. The coagulation-UV/H_2O_2 oxidation method resulted in much higher reduction rates for dissolved organic carbon(DOC)(by 75%) and UV_(254)(by 92%) than coagulation or UV/H_2O_2 oxidation alone. The proportion of non-acid hydrophobics, hydrophobic acids, transphilics and hydrophilics removed by coagulation was 54%, 49%, 27% and 12 %, while the combined treatment removed 92%, 87%,70% and 39%, respectively. Parallel factor analysis(PARAFAC) of fluorescence measurements revealed that the humic-like fluorescent component C4 showed the highest removal(by 44%)during the coagulation stage. After coagulation-UV/H_2O_2 treatment, the humic-like fluorescent component C3 had the highest removal(by 72%), whereas xenobiotic organic fluorescent components C1 and C4 remained recalcitrant to decomposition. Significant correlations(R2> 0.8)between C1 and the hydrophobic acids and non-acid hydrophobics suggested the possibility of using fluorescence spectroscopy as an effective tool to assess variations in DOM fraction treatment efficacy in coagulation-UV/H_2O_2 systems. After the combined treatment, toxic inhibition of cellular activity by post PhW W decreased from 88% to 47% and biodegradability increased from 0.1 to 0.52.
文摘制备了负载在Na Y分子筛上的Fe Cu Mn Y复合催化剂,并对其在非均相UV Fe Cu Mn Y H2O2体系中催化氧化4BS染料废水进行了研究.结果表明,非均相UV Fe Cu Mn Y H2O2体系对4BS染料废水的处理具有很高的效率.在基准条件下,反应时间为20min时,废水中4BS的去除率达到了93 7%.与均相UV Fenton体系不同,非均相UV Fe Cu Mn Y H2O2体系在碱性条件下(pH=10 5)仍可高效去除CODCr.动力学研究得到催化氧化4BS废水的模型方程,该模型可以为非均相UV Fe Cu Mn Y H2O2体系处理高色度的实际染料废水提供指导.
基金Project supported by the Science Project of Harbin City(No. H2001-12)the Youth Foundation of School of Municipal and Environmental Engineering in Harbin Institute of Technology(No. 01306914).
文摘The degradation of formaldehyde gas was studied using UV/TiO2/O3 process under the condition of continuous flow mode. The effects of humidity, initial formaldehyde concentration, residence time and ozone adding amount on degradation of formaldehyde gas were investigated. The experimental results indicated that the combination of ozonation with photocatalytic oxidation on the degradation of formaldehyde showed a synergetic action, e.g,, it could considerably increase decomposing of formaldehyde. The degradation efficiency of formaldehyde was between 73.6% and 79.4% while the initial concentration in the range of 1.84--24 mg/m^3 by O3/TiO2flJV process. The optimal humidity was about 50% in UV/TiO2/O3 processs and degradation of formaldehyde increases from 39.0% to 94.1% when the ozone content increased from 0 to 141 mg/m^3. Furthermore, the kinetics of formaldehyde degradation reaction could be described by Langmuir-Hinshelwood model. The rate constant k of 46.72 mg/（m^3.min） and Langmuir adsorption coefficient K of 0.0268 m^3/mg were obtained.
文摘In order to purify oil recovery wastewater from polymer flooding （ORWPF） in tertiary oil recovery in oil fields, advanced treatment of UV/H2O2/O3 and fine filtration were investigated. The experimental results showed that polyacrylamide and oil remaining in ORWPF after the conventional treatment process could be effectively removed by UV/H2O2/O3 process. Fine filtration gave a high performance in eliminating suspended solids. The treated ORWPF can meet the quality requirement of the wastewater-bearing polymer injection in oilfield and be safely re-injected into oil reservoirs for oil recovery.
