Developing low-cost and green simultaneous desulfurization and denitrification technologies is of great significance for sulfur dioxide(SO_(2))and nitrogen oxide(NO_(x))emission control at low temperatures,especially ...Developing low-cost and green simultaneous desulfurization and denitrification technologies is of great significance for sulfur dioxide(SO_(2))and nitrogen oxide(NO_(x))emission control at low temperatures,especially for small and medium-sized coal-fired boilers and furnaces.Herein,phosphorus sludge,an industrial waste from the production process of yellow phosphorus,has been developed to simultaneously eliminate SO_(2)and NO_(x)from coal-fired flue gas.The key factors affecting the experimental results indicate that desulfurization and denitrification efficiency of over 95%can be achieved at a low temperature of 55℃.Further,the absorption mechanism was investigated by characterizing the solid and liquid phases of the phosphorus sludge during the absorption process.The efficient removal of SO_(2)is attributed to the abundance of iron(Fe^(3+))and manganese(Mn^(2+))in the absorbent.SO_(2)can be rapidly catalyzed and converted to SO_(4)^(2-)by them.The key to NOx removal is the oxidation of NO toward watersoluble high-valent nitrogen oxides by oxidizing reactive substances induced via yellow phosphorus,which are then absorbed by water and converted to NO_(3)^(-).Meanwhile,yellow phosphorus is oxidized to phosphoric acid(H_(3)PO_(4)).The spent absorption slurry can be reused through wet process phosphoric acid production,as it contains sulfuric acid(H_(2)SO_(4)),nitric acid(HNO_(3)),and H_(3)PO_(4).Accordingly,this is a technology with broad application prospects.展开更多
Elucidating the effect of growth periods on the quality of calcium sulfate whiskers(CSWs)prepared from calcium sulfate dihydrate(DH)is imperative.Herein,crystal seeds and whiskers were prepared from DH in a water–gly...Elucidating the effect of growth periods on the quality of calcium sulfate whiskers(CSWs)prepared from calcium sulfate dihydrate(DH)is imperative.Herein,crystal seeds and whiskers were prepared from DH in a water–glycerol system.Longer whiskers were obtained from crystal seeds prepared via hydration of DH for 30 s than via ball milling for 5 min followed by hydration for 20 s.The attachment of cetyltrimethyl ammonium bromide and glycerol additives to the whisker tops promoted whisker growth.The whisker sponges exhibited good thermal barrier properties and compression cycle stability.展开更多
Phase change materials(PCMs)offer a promising solution to address the challenges posed by intermittency and fluctuations in solar thermal utilization.However,for organic solid-liquid PCMs,issues such as leakage,low th...Phase change materials(PCMs)offer a promising solution to address the challenges posed by intermittency and fluctuations in solar thermal utilization.However,for organic solid-liquid PCMs,issues such as leakage,low thermal conductivity,lack of efficient solar-thermal media,and flamma-bility have constrained their broad applications.Herein,we present an innova-tive class of versatile composite phase change materials(CPCMs)developed through a facile and environmentally friendly synthesis approach,leveraging the inherent anisotropy and unidirectional porosity of wood aerogel(nanowood)to support polyethylene glycol(PEG).The wood modification process involves the incorporation of phytic acid(PA)and MXene hybrid structure through an evaporation-induced assembly method,which could impart non-leaking PEG filling while concurrently facilitating thermal conduction,light absorption,and flame-retardant.Consequently,the as-prepared wood-based CPCMs showcase enhanced thermal conductivity(0.82 W m^(-1)K^(-1),about 4.6 times than PEG)as well as high latent heat of 135.5 kJ kg^(-1)(91.5%encapsula-tion)with thermal durability and stability throughout at least 200 heating and cooling cycles,featuring dramatic solar-thermal conversion efficiency up to 98.58%.In addition,with the synergistic effect of phytic acid and MXene,the flame-retardant performance of the CPCMs has been significantly enhanced,showing a self-extinguishing behavior.Moreover,the excellent electromagnetic shielding of 44.45 dB was endowed to the CPCMs,relieving contemporary health hazards associated with electromagnetic waves.Overall,we capitalize on the exquisite wood cell structure with unidirectional transport inherent in the development of multifunctional CPCMs,showcasing the operational principle through a proof-of-concept prototype system.展开更多
The keen interest in fuel cells and metal-air batteries stimulates a great deal of research on the development of a cost-efficient and high-performance catalyst as an alternative to traditional Pt to boost the sluggis...The keen interest in fuel cells and metal-air batteries stimulates a great deal of research on the development of a cost-efficient and high-performance catalyst as an alternative to traditional Pt to boost the sluggish oxygen reduction reaction(ORR)at the cathode.Herein,we report a facile and scalable strategy for the large-scale preparation of a free-standing and flexible porous atomically dispersed Fe-N-doped carbon microtube(FeSAC/PCMT)sponge.Benefiting from its unique structure that greatly facilitates the catalytic kinetics,mass transport,and electron transfer,our FeSAC/PCMT electrode exhibits excellent performance with an ORR potential of 0.942 V at^(-3) mA cm^(-2).When the FeSAC/PCMT sponge was directly used as an oxygen electrode for liquid-state and flexible solid-state zinc-air batteries,high peak power densities of 183.1 and 58.0 mW cm^(-2) were respectively achieved,better than its powdery counterpart and commercial Pt/C catalyst.Experimental and theoretical investigation results demonstrate that such ultrahigh ORR performance can be attributed to atomically dispersed Fe-N_(5) species in FeSAC/PCMT.This study presents a cost-effective and scalable strategy for the fabrication of highly efficient and flexible oxygen electrodes,provides a significant new insight into the catalytic mechanisms,and helps to realize significant advances in energy devices.展开更多
目的探讨股前外侧皮瓣修复重建后口腔癌患者生存质量的影响因素。方法选取本院2014年6月至2017年6月收治的口腔癌患者103例为研究对象,所有患者均行口腔癌根治术和股前外侧皮瓣修复重建。采用汉化第4版华盛顿大学生存质量问卷(universit...目的探讨股前外侧皮瓣修复重建后口腔癌患者生存质量的影响因素。方法选取本院2014年6月至2017年6月收治的口腔癌患者103例为研究对象,所有患者均行口腔癌根治术和股前外侧皮瓣修复重建。采用汉化第4版华盛顿大学生存质量问卷(universityof Washington quality of life,UW-QOL)进行访谈式自评调查回访评价患者术后12个月的生存质量,采用单因素和多因素Logistic回归分析探讨股前外侧皮瓣修复重建后口腔癌患者生存质量的影响因素。结果年龄、肿瘤分期、术后是否放疗、术后有无复发、颈淋巴清扫术均为股前外侧皮瓣修复重建后口腔癌患者生存质量的影响因素(P_均<0.05),其中年龄≥50岁、肿瘤分期T_3~T_4期、术后放疗、术后复发及根治性颈淋巴清扫术均为影响股前外侧皮瓣修复重建后口腔癌患者生存质量的独立危险因素(P_均<0.05)。结论股前外侧皮瓣修复重建后口腔癌患者生存质量受多种影响因素,应针对各危险因素采取相应干预措施,提高患者生存质量。展开更多
Land use change is one of the major factors that affect soil organic carbon （SOC） variation and global carbon balance. However, the effects of land use change on SOC are always variable. In this study, using a serie...Land use change is one of the major factors that affect soil organic carbon （SOC） variation and global carbon balance. However, the effects of land use change on SOC are always variable. In this study, using a series of paired-field experiments, we estimated the effects of revegetation types and environmental conditions on SOC stock and vertical distribution after replacement of cropland with poplar （Populus tomentosa） and korshinsk peashrub （Caragana korshinskt＇i） in three climate regions （Chifeng City, Fengning City and Datong City of the ＇Beijing-Tianjin Sandstorm Source Control＇ （BTSSC） program area. The results show that SOC sequestration rate ranges from 0.15 Mg/（ha-yr） to 3.76 Mg/（ha-yr） in the soil layer of 0-100 cm in early stage after cropland afforestation in the BTSSC program area. The SOC accumulation rates are the highest in Fengning for both the two vegetation types. Compared to C. korshinskii, P tomentosa has greater effects on SOC accumulation in the three climate regions, but significantly greater effect only appears in Datong. The SOC density increases by 20%-111% and 15%-59% for P. tomentosa and 9%-63% and 0-73% for C. korshinskii in the 0-20 cm and 20-100 cm soil layers, respectively. Our results indicate that cropland afforestation not only affects SOC stock in the topsoil, but also has some effects on subsoil carbon. However, the effect of cropland afforestation on SOC accumulation varied with climate regions and revegetation types. Considering the large area of revegetation and relatively high SOC accumulation rate, SOC sequestration in the BTSSC program should contribute significantly to decrease the CO2 concentration in the atmosphere.展开更多
In order to better understand the compositional and structural complexity of dissolved organic matter(DOM) macromolecules and provide mechanistic information on the binding of hydrophobic organic contaminants(HOCs) to...In order to better understand the compositional and structural complexity of dissolved organic matter(DOM) macromolecules and provide mechanistic information on the binding of hydrophobic organic contaminants(HOCs) to DOM, we fractionated large amounts of lake water into three hydrophobic DOM-fractions. The variation of the partitioning coef?cients(K_(DOC)) of pyrene at different p H levels was examined by ?orescence quenching titration. Results show that, relative to the more polar acidic DOM-fractions, the hydrophobic neutral fraction exhibits a higher sorption ability to pyrene. Generally, the sorption of pyrene to the three hydrophobic fractions is strongly pH-dependent. The K_(DOC) values of pyrene generally increase with decreasing p H levels, which is especially obvious in the sorption of pyrene to the fulvic acid fractions, suggesting that the binding is controlled by hydrophobic interactions. The mechanisms underlying the binding of pyrene to the hydrophobic fractions were also discussed. Our data are bene?cial to further understanding the binding of HOCs to DOM and how it has been affected,which may result in more accurate predictions of K_(DOC).展开更多
The cognition of active sites in the Ni-based catalysts plays a vital role and remains a huge challenge in improving catalytic performance of low temperature CO_(2) dry reforming of methane(LTDRM).In this work,typical...The cognition of active sites in the Ni-based catalysts plays a vital role and remains a huge challenge in improving catalytic performance of low temperature CO_(2) dry reforming of methane(LTDRM).In this work,typical catalysts of SiO_(2) and γ-Al_(2)O_(3) supported Ni and Ni-Ce were designed and prepared.Importantly,the difference in the chemical speciations of active sites on the Ni-based catalysts is revealed by advanced characterizations and further estimates respective catalytic performance for LTDRM.Results show that larger[Ni0-]particles mixed with[Ni-O-Sin])species on the Ni/SiO_(2)(R)make CH_(4) excessive decomposition,leading to poor activity and stability.Once the Ce species is doped,however,superior activity(59.0%CH_(4) and 59.8%CO_(2) conversions),stability and high H_(2)/CO ratio(0.96)at 600℃ can be achieved on the Ni-Ce/SiO_(2)(R),in comparison with other catalysts and even reported studies.The improved performance can be ascribed to the formation of integral([Ni0_(n))]-[CeⅢ-□-CeⅢ])species on the Ni-Ce/SiO_(2)(R)catalyst,containing highly dispersed[Ni]particles and rich oxygen vacancies,which can synergistically establish a new stable balance between gasification of carbon species and CO_(2) dissocia-tion.With respect to Ni-Ce/γ-Al_(2)O_(3)(R),the Ni and Ce precursors are easily captured by extra-framework Al_(n)-OH groups and further form stable isolated([Ni0_(n))]-[Ni-O-Al_(n)])and[CeⅢ-O-Al_(n)]species.In such a case,both of them preferentially accelerate CO_(2) adsorption and dissociation,causing more car-bon deposition due to the disproportionation of superfuous CO product.This deep distinguishment of chemical speciations of active sites can guide us to further develop new efficient Ni-based catalysts for LTDRM in the future.展开更多
基金The National Natural Science Foundation of China (22068019)Yunnan Major Scientific and Technological Projects (202202AG050001)
文摘Developing low-cost and green simultaneous desulfurization and denitrification technologies is of great significance for sulfur dioxide(SO_(2))and nitrogen oxide(NO_(x))emission control at low temperatures,especially for small and medium-sized coal-fired boilers and furnaces.Herein,phosphorus sludge,an industrial waste from the production process of yellow phosphorus,has been developed to simultaneously eliminate SO_(2)and NO_(x)from coal-fired flue gas.The key factors affecting the experimental results indicate that desulfurization and denitrification efficiency of over 95%can be achieved at a low temperature of 55℃.Further,the absorption mechanism was investigated by characterizing the solid and liquid phases of the phosphorus sludge during the absorption process.The efficient removal of SO_(2)is attributed to the abundance of iron(Fe^(3+))and manganese(Mn^(2+))in the absorbent.SO_(2)can be rapidly catalyzed and converted to SO_(4)^(2-)by them.The key to NOx removal is the oxidation of NO toward watersoluble high-valent nitrogen oxides by oxidizing reactive substances induced via yellow phosphorus,which are then absorbed by water and converted to NO_(3)^(-).Meanwhile,yellow phosphorus is oxidized to phosphoric acid(H_(3)PO_(4)).The spent absorption slurry can be reused through wet process phosphoric acid production,as it contains sulfuric acid(H_(2)SO_(4)),nitric acid(HNO_(3)),and H_(3)PO_(4).Accordingly,this is a technology with broad application prospects.
基金supported by the Degradable Plastics Engineering Research Center of Yunnan Provincial Education Department(KKPU202205001).
文摘Elucidating the effect of growth periods on the quality of calcium sulfate whiskers(CSWs)prepared from calcium sulfate dihydrate(DH)is imperative.Herein,crystal seeds and whiskers were prepared from DH in a water–glycerol system.Longer whiskers were obtained from crystal seeds prepared via hydration of DH for 30 s than via ball milling for 5 min followed by hydration for 20 s.The attachment of cetyltrimethyl ammonium bromide and glycerol additives to the whisker tops promoted whisker growth.The whisker sponges exhibited good thermal barrier properties and compression cycle stability.
基金funding from the National Natural Science Foundation of China(No.22268025)China Postdoctoral Science Foundation(NO.2022MD713757)+2 种基金Yunnan Provincial Postdoctoral Science Foundation(NO.34Y2022)Yunnan Province Joint Special Project for Enterprise Fundamental Research and Applied Basic Research(No.202101BC070001-016)Guangdong Basic and Applied Basic Research Foundation(No.2023A1515011985).
文摘Phase change materials(PCMs)offer a promising solution to address the challenges posed by intermittency and fluctuations in solar thermal utilization.However,for organic solid-liquid PCMs,issues such as leakage,low thermal conductivity,lack of efficient solar-thermal media,and flamma-bility have constrained their broad applications.Herein,we present an innova-tive class of versatile composite phase change materials(CPCMs)developed through a facile and environmentally friendly synthesis approach,leveraging the inherent anisotropy and unidirectional porosity of wood aerogel(nanowood)to support polyethylene glycol(PEG).The wood modification process involves the incorporation of phytic acid(PA)and MXene hybrid structure through an evaporation-induced assembly method,which could impart non-leaking PEG filling while concurrently facilitating thermal conduction,light absorption,and flame-retardant.Consequently,the as-prepared wood-based CPCMs showcase enhanced thermal conductivity(0.82 W m^(-1)K^(-1),about 4.6 times than PEG)as well as high latent heat of 135.5 kJ kg^(-1)(91.5%encapsula-tion)with thermal durability and stability throughout at least 200 heating and cooling cycles,featuring dramatic solar-thermal conversion efficiency up to 98.58%.In addition,with the synergistic effect of phytic acid and MXene,the flame-retardant performance of the CPCMs has been significantly enhanced,showing a self-extinguishing behavior.Moreover,the excellent electromagnetic shielding of 44.45 dB was endowed to the CPCMs,relieving contemporary health hazards associated with electromagnetic waves.Overall,we capitalize on the exquisite wood cell structure with unidirectional transport inherent in the development of multifunctional CPCMs,showcasing the operational principle through a proof-of-concept prototype system.
基金supported by the start-up fund from Kunming University of Science and Technology,the National Natural Science Foundation of China (Grants 52102046,51872293,52130209,52072375)Liaoning Revitalization Talents Program (XLYC2002037)Basic Research Project of Natural Science Foundation of Shandong Province,China (ZR2019ZD49).
文摘The keen interest in fuel cells and metal-air batteries stimulates a great deal of research on the development of a cost-efficient and high-performance catalyst as an alternative to traditional Pt to boost the sluggish oxygen reduction reaction(ORR)at the cathode.Herein,we report a facile and scalable strategy for the large-scale preparation of a free-standing and flexible porous atomically dispersed Fe-N-doped carbon microtube(FeSAC/PCMT)sponge.Benefiting from its unique structure that greatly facilitates the catalytic kinetics,mass transport,and electron transfer,our FeSAC/PCMT electrode exhibits excellent performance with an ORR potential of 0.942 V at^(-3) mA cm^(-2).When the FeSAC/PCMT sponge was directly used as an oxygen electrode for liquid-state and flexible solid-state zinc-air batteries,high peak power densities of 183.1 and 58.0 mW cm^(-2) were respectively achieved,better than its powdery counterpart and commercial Pt/C catalyst.Experimental and theoretical investigation results demonstrate that such ultrahigh ORR performance can be attributed to atomically dispersed Fe-N_(5) species in FeSAC/PCMT.This study presents a cost-effective and scalable strategy for the fabrication of highly efficient and flexible oxygen electrodes,provides a significant new insight into the catalytic mechanisms,and helps to realize significant advances in energy devices.
文摘目的探讨股前外侧皮瓣修复重建后口腔癌患者生存质量的影响因素。方法选取本院2014年6月至2017年6月收治的口腔癌患者103例为研究对象,所有患者均行口腔癌根治术和股前外侧皮瓣修复重建。采用汉化第4版华盛顿大学生存质量问卷(universityof Washington quality of life,UW-QOL)进行访谈式自评调查回访评价患者术后12个月的生存质量,采用单因素和多因素Logistic回归分析探讨股前外侧皮瓣修复重建后口腔癌患者生存质量的影响因素。结果年龄、肿瘤分期、术后是否放疗、术后有无复发、颈淋巴清扫术均为股前外侧皮瓣修复重建后口腔癌患者生存质量的影响因素(P_均<0.05),其中年龄≥50岁、肿瘤分期T_3~T_4期、术后放疗、术后复发及根治性颈淋巴清扫术均为影响股前外侧皮瓣修复重建后口腔癌患者生存质量的独立危险因素(P_均<0.05)。结论股前外侧皮瓣修复重建后口腔癌患者生存质量受多种影响因素,应针对各危险因素采取相应干预措施,提高患者生存质量。
基金Under the auspices of Strategic Priority Research Program of Chinese Academy of Sciences(No.XDA05060600)Knowledge Innovation Programs of Chinese Academy of Sciences(No.KSCX2-EW-J-5)National Key Technology Research and Development Program of China(No.2011BAD31B02)
文摘Land use change is one of the major factors that affect soil organic carbon （SOC） variation and global carbon balance. However, the effects of land use change on SOC are always variable. In this study, using a series of paired-field experiments, we estimated the effects of revegetation types and environmental conditions on SOC stock and vertical distribution after replacement of cropland with poplar （Populus tomentosa） and korshinsk peashrub （Caragana korshinskt＇i） in three climate regions （Chifeng City, Fengning City and Datong City of the ＇Beijing-Tianjin Sandstorm Source Control＇ （BTSSC） program area. The results show that SOC sequestration rate ranges from 0.15 Mg/（ha-yr） to 3.76 Mg/（ha-yr） in the soil layer of 0-100 cm in early stage after cropland afforestation in the BTSSC program area. The SOC accumulation rates are the highest in Fengning for both the two vegetation types. Compared to C. korshinskii, P tomentosa has greater effects on SOC accumulation in the three climate regions, but significantly greater effect only appears in Datong. The SOC density increases by 20%-111% and 15%-59% for P. tomentosa and 9%-63% and 0-73% for C. korshinskii in the 0-20 cm and 20-100 cm soil layers, respectively. Our results indicate that cropland afforestation not only affects SOC stock in the topsoil, but also has some effects on subsoil carbon. However, the effect of cropland afforestation on SOC accumulation varied with climate regions and revegetation types. Considering the large area of revegetation and relatively high SOC accumulation rate, SOC sequestration in the BTSSC program should contribute significantly to decrease the CO2 concentration in the atmosphere.
基金supported by the National Natural Science Foundation of China (No. 41173128)
文摘In order to better understand the compositional and structural complexity of dissolved organic matter(DOM) macromolecules and provide mechanistic information on the binding of hydrophobic organic contaminants(HOCs) to DOM, we fractionated large amounts of lake water into three hydrophobic DOM-fractions. The variation of the partitioning coef?cients(K_(DOC)) of pyrene at different p H levels was examined by ?orescence quenching titration. Results show that, relative to the more polar acidic DOM-fractions, the hydrophobic neutral fraction exhibits a higher sorption ability to pyrene. Generally, the sorption of pyrene to the three hydrophobic fractions is strongly pH-dependent. The K_(DOC) values of pyrene generally increase with decreasing p H levels, which is especially obvious in the sorption of pyrene to the fulvic acid fractions, suggesting that the binding is controlled by hydrophobic interactions. The mechanisms underlying the binding of pyrene to the hydrophobic fractions were also discussed. Our data are bene?cial to further understanding the binding of HOCs to DOM and how it has been affected,which may result in more accurate predictions of K_(DOC).
基金financially supported by the National Natural Science Foundation of China (22006059, 21968015)National Engineering Laboratory for Flue Gas Pollutants Control Technology and Equipment (NEL-KF-201905)+1 种基金Applied Basic Research Program of Yunnan Province, China (202101AU070154, 2019FD034)Analysis and Testing Fund of Kunming University of Science and Technology (2020 T20200006)
文摘The cognition of active sites in the Ni-based catalysts plays a vital role and remains a huge challenge in improving catalytic performance of low temperature CO_(2) dry reforming of methane(LTDRM).In this work,typical catalysts of SiO_(2) and γ-Al_(2)O_(3) supported Ni and Ni-Ce were designed and prepared.Importantly,the difference in the chemical speciations of active sites on the Ni-based catalysts is revealed by advanced characterizations and further estimates respective catalytic performance for LTDRM.Results show that larger[Ni0-]particles mixed with[Ni-O-Sin])species on the Ni/SiO_(2)(R)make CH_(4) excessive decomposition,leading to poor activity and stability.Once the Ce species is doped,however,superior activity(59.0%CH_(4) and 59.8%CO_(2) conversions),stability and high H_(2)/CO ratio(0.96)at 600℃ can be achieved on the Ni-Ce/SiO_(2)(R),in comparison with other catalysts and even reported studies.The improved performance can be ascribed to the formation of integral([Ni0_(n))]-[CeⅢ-□-CeⅢ])species on the Ni-Ce/SiO_(2)(R)catalyst,containing highly dispersed[Ni]particles and rich oxygen vacancies,which can synergistically establish a new stable balance between gasification of carbon species and CO_(2) dissocia-tion.With respect to Ni-Ce/γ-Al_(2)O_(3)(R),the Ni and Ce precursors are easily captured by extra-framework Al_(n)-OH groups and further form stable isolated([Ni0_(n))]-[Ni-O-Al_(n)])and[CeⅢ-O-Al_(n)]species.In such a case,both of them preferentially accelerate CO_(2) adsorption and dissociation,causing more car-bon deposition due to the disproportionation of superfuous CO product.This deep distinguishment of chemical speciations of active sites can guide us to further develop new efficient Ni-based catalysts for LTDRM in the future.
