The hydrogen isotopic composition(δD) of leaf wax long-chain n-alkanes(C27, C29, and C31) from lacustrine sediments has been widely applied to reconstruct terrestrial paleoclimatic and paleohydrological changes. Howe...The hydrogen isotopic composition(δD) of leaf wax long-chain n-alkanes(C27, C29, and C31) from lacustrine sediments has been widely applied to reconstruct terrestrial paleoclimatic and paleohydrological changes. However, few studies have addressed whether the aquatic-derived n-alkanes can affect the δD values of lake sedimentary long-chain n-alkanes, which are usually regarded as a recorder of the terrestrial hydrological signals. Here we systematically investigated δD values of long-chain n-alkanes from modern aquatic plants, both near-shore and off-shore surface sediments, surrounding terrestrial plant litters, as well as river water and lake water in Lake Qinghai and its satellite lakes on the northeastern Qinghai-Tibet Plateau. Our data showed that(i) δD values of long-chain n-alkanes from aquatic plants varied from-184‰ to-132‰ for n-C27, from-183‰ to-138‰ for n-C29, and from-189‰ to-130‰ for n-C31, respectively, with no significant differences among the three n-alkanes homologues;(ii) δD values of long-chain n-alkanes from aquatic plants were generally more positive than those from surrounding terrestrial plants, possibly because that they recorded the D-enrichment of lake water in this semi-arid region;(iii) δD values of long-chain n-alkanes from surface sediments showed significant differences among the three n-alkanes homologues, due to the larger aquatic input of n-C27 to the sedimentary lipid pool than that of n-C31, and(iv) n-C27 δD values of near-shore aquatic plants and near-shore sediments are more negative than those from off-shore as a result of lower δD values of near-shore lake water. Our findings indicate that in this region(i) the offset between sedimentary n-C27 and n-C31 δD values(ΔδDC27-C31) could potentially be used to evaluate if sedimentary long-chain n-alkanes are derived from a single source;(ii) while δD values of n-C27 may be influenced by lake water hydrological changes, sedimentary n-C31 is derived predominantly from terrestrial plants and thus its δD can 展开更多
To investigate characteristics of H isotope variation in long-chain n-alkanes （δDn-alkanes） from higher plants in surface soils under a single ecosystem, 12 samples from a basalt regolith were randomly collected fr...To investigate characteristics of H isotope variation in long-chain n-alkanes （δDn-alkanes） from higher plants in surface soils under a single ecosystem, 12 samples from a basalt regolith were randomly collected from Damaping in Wanquan County of Zhangjiakou in North China. Molecular distribution and C （δ^13Cn-alkanes） and H isotopes of long-chain n-alkanes, as well as C isotopes of TOC （δ^13CTOC）, were analyzed. Both δ^13CTOC and δ^13Cn-alkanes values from four representative dominant long-chain n-alkanes （n-C27, n-C29, n-C31, n-C33） derived from terrestrial higher plants show minor variations among the 12 samples, indicating the major contributor is from local grasses with a uniform C3 photosynthetic pathway. In contrast, variations in δ^13Cn-alkanes values of the four long-chain n-alkanes are relatively large, with the more abundant homologs generally showing more negative δDn-alkanes values and less variation. However, variation of 〈30‰ among weighted averaged δDn-alkanes values of the four long-chain n-alkanes is not only less than that among δDn-alkanes values for different modern terrestrial C3 grasses from the specific locations, but also less than the literature values of δDn-alkanes of long-chain n-alkanes for single species over different seasons. Thus, because the sources of long-chain n-alkanes in surface soils and sediments are similarly from multiple individual plants, our results are significant in confirming that paleoclimatic, paleoenvironmental and paleohydrological information can be interpreted more accurately from δDn-alkanes values of long-chain n-alkanes from sediments, particularly terrestrial sediments with organic matter derived from in-situ plants.展开更多
Long-chain alkanes are abundant feedstocks supplied by natural resources and chemical industry. Specially, normal long-chain alkanes are primary products from Fischer-Tropsch synthesis(FTS) process, which is an import...Long-chain alkanes are abundant feedstocks supplied by natural resources and chemical industry. Specially, normal long-chain alkanes are primary products from Fischer-Tropsch synthesis(FTS) process, which is an important route for the utilization of coal in China. Facing a shift of energy nexus towards sustainable society, the conversion of long-chain alkanes derived from coal into value-added products(such as alkenes and oxygenates) is of great importance for securing China’s energy supply and the role transition of the commercial FTS plants from fuel makers to chemical suppliers. Among the potential transformation routes,the direct dehydrogenation of long-chain alkanes into alkenes is an attractive and practical route, due to the broad applications of long-chain alkenes(especially the linear α-olefins). In this review, we will summary the key insights obtained from the literature on the dehydrogenation of light alkanes based on supported metal catalysts and the dehydrogenation of alkanes with homogeneous molecular catalysts and then discuss how to translate these lessons into the development of efficient catalysts and processes for the dehydrogenation of long-chain alkanes into long-chain alkenes.展开更多
Long-chain n-alkanols and n-alkanes in core sediments from the northern South China Sea(SCS)were measured to make a comparison during terrestrial vegetation reconstruction from~42 ka to~7 ka.The results showed that te...Long-chain n-alkanols and n-alkanes in core sediments from the northern South China Sea(SCS)were measured to make a comparison during terrestrial vegetation reconstruction from~42 ka to~7 ka.The results showed that terrestrial vegetation record from long-chain n-alkanes matched well with previous studies in nearby cores,showing that more C_(4)plants developed during the Last Glacial Maximum(LGM)and C_(3)plants dominated in the interglacial period.However,these scenarios were not revealed by terrestrial vegetation reconstruction using long-chain n-alkanols,which showed C_(3)plant expansion during the LGM.The discrepancy during the interglacial period could be attributed to the aerobic degradation of functionalized long-chain n-alkanols in the oxygen-rich bottom water,resulting in poor preservation of terrestrial vegetation signals.On the other hand,the different advantages of functionalized n-alkanols and non-functional n-alkanes to record local and distal vegetation signals,respectively,may offer a potential explanation for the contradiction during the LGM when the SCS was characterized by low-oxygen deep water.Nevertheless,large variations on n-alkyl lipid compositions in C_(3)/C_(4)plants could play a part in modulating sedimentary long-chain n-alkanols and n-alkanes toward different vegetation signals,thereby suggesting that caution must be taken in respect to the terrestrial vegetation reconstruction using long-chain n-alkanes and long-chain n-alkanols.展开更多
Fatty acids with different chain length were deoxygenated in the absence of hydrogen (caprylic acid (CA), lauric acid (LA) and stearic acid (SA)). The catalytic tests were carried over Pd-containing catalysts out in a...Fatty acids with different chain length were deoxygenated in the absence of hydrogen (caprylic acid (CA), lauric acid (LA) and stearic acid (SA)). The catalytic tests were carried over Pd-containing catalysts out in a batch reactor under inert gas for 6 h at 250°C to 350°C and pressures from 18 to 75 bar in the absence of additionally fed hydrogen. Pd-containing catalysts were tested;the best performing catalyst was 10% Pd/C with 63% undecane yield at 327°C. These catalysts were used for a comparative decarboxylation of CA, LA and SA. At equal reaction conditions (300°C, 6 h), the chain length of the fatty acid had a strong impact on the conversion, which was steadily increasing, whereas the alkane selectivity ran through a maximum. This work demonstrated the usability of Pd-containing catalysts for the decarboxylation of various fatty acids in the absence of additionally fed hydrogen with respect to the manufacture of hydrocarbons that can be used as blending components for fuels.展开更多
As a representative species of intermediate volatile organic compounds(IVOCs),long-chain alkanes are considered to be important precursors of secondary organic aerosols(SOA)in the atmosphere.This work reviews the prev...As a representative species of intermediate volatile organic compounds(IVOCs),long-chain alkanes are considered to be important precursors of secondary organic aerosols(SOA)in the atmosphere.This work reviews the previous studies on long-chain alkanes in the atmosphere:(1)the detection methods and filed observations of long-chain alkanes in both gas and particle phases are summarized briefly;(2)the laboratory studies of long chain alkanes are reviewed,the kinetic data,reaction mechanism,SOA yields,and physicochemical properties of SOA are included in detail;(3)the research progress related to model simulations of long-chain alkanes are also discussed.In addition,based on available research results,several perspective contents are proposed that can be used as a guideline for future research plans.展开更多
The molecular distribution of long-chain n-alkanes in 62 soil samples collected from diverse locations across eastern China was analyzed.The long-chain n-alkanes were mostly dominated by n-C29 or n-C31,regardless of t...The molecular distribution of long-chain n-alkanes in 62 soil samples collected from diverse locations across eastern China was analyzed.The long-chain n-alkanes were mostly dominated by n-C29 or n-C31,regardless of the overlying vegetation type at each site.The results were compared with those summarized from the literature,covering more than 100 soil samples within China and more than 300 genera of modern plants distributed worldwide.There were similar n-alkane distribution patterns for most genera, with no clear differences among grasses,shrubs,and trees.The evidence from analyses of surface soils and modern plants indicates that the relationship between the molecular distribution of long-chain n-alkanes of surface soils and source vegetation is highly complex,and is influenced by many factors.Further,it is suggested that source vegetation types should not be simply inferred from distribution patterns of long-chain n-alkanes in sediments.展开更多
基金supported by the National Natural Science Foundation of China (Grant No. 41573005)the National Basic Research Program of China (Grant No. 2013CB955901)
文摘The hydrogen isotopic composition(δD) of leaf wax long-chain n-alkanes(C27, C29, and C31) from lacustrine sediments has been widely applied to reconstruct terrestrial paleoclimatic and paleohydrological changes. However, few studies have addressed whether the aquatic-derived n-alkanes can affect the δD values of lake sedimentary long-chain n-alkanes, which are usually regarded as a recorder of the terrestrial hydrological signals. Here we systematically investigated δD values of long-chain n-alkanes from modern aquatic plants, both near-shore and off-shore surface sediments, surrounding terrestrial plant litters, as well as river water and lake water in Lake Qinghai and its satellite lakes on the northeastern Qinghai-Tibet Plateau. Our data showed that(i) δD values of long-chain n-alkanes from aquatic plants varied from-184‰ to-132‰ for n-C27, from-183‰ to-138‰ for n-C29, and from-189‰ to-130‰ for n-C31, respectively, with no significant differences among the three n-alkanes homologues;(ii) δD values of long-chain n-alkanes from aquatic plants were generally more positive than those from surrounding terrestrial plants, possibly because that they recorded the D-enrichment of lake water in this semi-arid region;(iii) δD values of long-chain n-alkanes from surface sediments showed significant differences among the three n-alkanes homologues, due to the larger aquatic input of n-C27 to the sedimentary lipid pool than that of n-C31, and(iv) n-C27 δD values of near-shore aquatic plants and near-shore sediments are more negative than those from off-shore as a result of lower δD values of near-shore lake water. Our findings indicate that in this region(i) the offset between sedimentary n-C27 and n-C31 δD values(ΔδDC27-C31) could potentially be used to evaluate if sedimentary long-chain n-alkanes are derived from a single source;(ii) while δD values of n-C27 may be influenced by lake water hydrological changes, sedimentary n-C31 is derived predominantly from terrestrial plants and thus its δD can
基金supported by the National Natural Science Foundation of China (Grant Nos. 40901055 and 40872111)the Key Program of Chinese Ministry of Education (Grant No. 109151)+1 种基金the National Basic Research Program of China (Grant No. 2010CB950202)the NSFC National Innovative Research Team Project (Grant No. 41021091)
文摘To investigate characteristics of H isotope variation in long-chain n-alkanes （δDn-alkanes） from higher plants in surface soils under a single ecosystem, 12 samples from a basalt regolith were randomly collected from Damaping in Wanquan County of Zhangjiakou in North China. Molecular distribution and C （δ^13Cn-alkanes） and H isotopes of long-chain n-alkanes, as well as C isotopes of TOC （δ^13CTOC）, were analyzed. Both δ^13CTOC and δ^13Cn-alkanes values from four representative dominant long-chain n-alkanes （n-C27, n-C29, n-C31, n-C33） derived from terrestrial higher plants show minor variations among the 12 samples, indicating the major contributor is from local grasses with a uniform C3 photosynthetic pathway. In contrast, variations in δ^13Cn-alkanes values of the four long-chain n-alkanes are relatively large, with the more abundant homologs generally showing more negative δDn-alkanes values and less variation. However, variation of 〈30‰ among weighted averaged δDn-alkanes values of the four long-chain n-alkanes is not only less than that among δDn-alkanes values for different modern terrestrial C3 grasses from the specific locations, but also less than the literature values of δDn-alkanes of long-chain n-alkanes for single species over different seasons. Thus, because the sources of long-chain n-alkanes in surface soils and sediments are similarly from multiple individual plants, our results are significant in confirming that paleoclimatic, paleoenvironmental and paleohydrological information can be interpreted more accurately from δDn-alkanes values of long-chain n-alkanes from sediments, particularly terrestrial sediments with organic matter derived from in-situ plants.
基金supported by Tsinghua University(Initiative Scientific Research Program 20211080079)the National Natural Science Foundation of China(21972161,22172186)+7 种基金Chinese Academy of Sciences(CAS)Pioneer Talents Program(2018-095)Shanxi Talent Program(2019SBRJH01)Autonomous Research Project of State Key Laboratory of Coal Conversion(SKLCC)(2020BWZ006,2021BWZ007)Institute of Coal Chemistry(ICC)Innovation Fund(SCJJ-2020-02)Inner Mengolia Science&Technology Project Plan(2021GG0311)Major science and technology project of Ordos(2022EEDSKJZDZX001)Start-Up Grant of Institute of Coal Chemistry(2020SC001)Synfuels China Co.,Ltd.
文摘Long-chain alkanes are abundant feedstocks supplied by natural resources and chemical industry. Specially, normal long-chain alkanes are primary products from Fischer-Tropsch synthesis(FTS) process, which is an important route for the utilization of coal in China. Facing a shift of energy nexus towards sustainable society, the conversion of long-chain alkanes derived from coal into value-added products(such as alkenes and oxygenates) is of great importance for securing China’s energy supply and the role transition of the commercial FTS plants from fuel makers to chemical suppliers. Among the potential transformation routes,the direct dehydrogenation of long-chain alkanes into alkenes is an attractive and practical route, due to the broad applications of long-chain alkenes(especially the linear α-olefins). In this review, we will summary the key insights obtained from the literature on the dehydrogenation of light alkanes based on supported metal catalysts and the dehydrogenation of alkanes with homogeneous molecular catalysts and then discuss how to translate these lessons into the development of efficient catalysts and processes for the dehydrogenation of long-chain alkanes into long-chain alkenes.
基金The Key Special Project for Introduced Talents Team of Southern Marine Science and Engineering Guangdong Laboratory(Guangzhou)under contract No.GML2019ZD0104the Science and Technology Program of Guangzhou,China under contract No.201804010264+3 种基金the Guangdong MEPP Fund under contract No.GDOE[2019]A41the National Natural Science Foundation of China under contract No.41706059the Fund of Institution of South China Sea Ecology and Environmental Engineering,Chinese Academy of Sciences under contract No.ISEE2020YB05the State Key R&D Project under contract No.2016YFA0601104。
文摘Long-chain n-alkanols and n-alkanes in core sediments from the northern South China Sea(SCS)were measured to make a comparison during terrestrial vegetation reconstruction from~42 ka to~7 ka.The results showed that terrestrial vegetation record from long-chain n-alkanes matched well with previous studies in nearby cores,showing that more C_(4)plants developed during the Last Glacial Maximum(LGM)and C_(3)plants dominated in the interglacial period.However,these scenarios were not revealed by terrestrial vegetation reconstruction using long-chain n-alkanols,which showed C_(3)plant expansion during the LGM.The discrepancy during the interglacial period could be attributed to the aerobic degradation of functionalized long-chain n-alkanols in the oxygen-rich bottom water,resulting in poor preservation of terrestrial vegetation signals.On the other hand,the different advantages of functionalized n-alkanols and non-functional n-alkanes to record local and distal vegetation signals,respectively,may offer a potential explanation for the contradiction during the LGM when the SCS was characterized by low-oxygen deep water.Nevertheless,large variations on n-alkyl lipid compositions in C_(3)/C_(4)plants could play a part in modulating sedimentary long-chain n-alkanols and n-alkanes toward different vegetation signals,thereby suggesting that caution must be taken in respect to the terrestrial vegetation reconstruction using long-chain n-alkanes and long-chain n-alkanols.
文摘Fatty acids with different chain length were deoxygenated in the absence of hydrogen (caprylic acid (CA), lauric acid (LA) and stearic acid (SA)). The catalytic tests were carried over Pd-containing catalysts out in a batch reactor under inert gas for 6 h at 250°C to 350°C and pressures from 18 to 75 bar in the absence of additionally fed hydrogen. Pd-containing catalysts were tested;the best performing catalyst was 10% Pd/C with 63% undecane yield at 327°C. These catalysts were used for a comparative decarboxylation of CA, LA and SA. At equal reaction conditions (300°C, 6 h), the chain length of the fatty acid had a strong impact on the conversion, which was steadily increasing, whereas the alkane selectivity ran through a maximum. This work demonstrated the usability of Pd-containing catalysts for the decarboxylation of various fatty acids in the absence of additionally fed hydrogen with respect to the manufacture of hydrocarbons that can be used as blending components for fuels.
基金supported by the Postdoctoral Research Foundation of China(No.2019M660752)Beijing Municipal Commission of Education(No.Z181100005418015)the National Natural Science Foundation of China(Nos.91744204,41822703)
文摘As a representative species of intermediate volatile organic compounds(IVOCs),long-chain alkanes are considered to be important precursors of secondary organic aerosols(SOA)in the atmosphere.This work reviews the previous studies on long-chain alkanes in the atmosphere:(1)the detection methods and filed observations of long-chain alkanes in both gas and particle phases are summarized briefly;(2)the laboratory studies of long chain alkanes are reviewed,the kinetic data,reaction mechanism,SOA yields,and physicochemical properties of SOA are included in detail;(3)the research progress related to model simulations of long-chain alkanes are also discussed.In addition,based on available research results,several perspective contents are proposed that can be used as a guideline for future research plans.
基金supported by the National Natural Science Foundation of China (40901055)the Key Project of the Chinese Ministry of Education (109151)+2 种基金the Fund for Creative Research Groups (41021091)the Cross-discipline Innovative Study Fund for Youth Talent of Lanzhou University (LZUJC2007011)the National Basic Research Program of China (2010CB950202 and 2010CB833405)
文摘The molecular distribution of long-chain n-alkanes in 62 soil samples collected from diverse locations across eastern China was analyzed.The long-chain n-alkanes were mostly dominated by n-C29 or n-C31,regardless of the overlying vegetation type at each site.The results were compared with those summarized from the literature,covering more than 100 soil samples within China and more than 300 genera of modern plants distributed worldwide.There were similar n-alkane distribution patterns for most genera, with no clear differences among grasses,shrubs,and trees.The evidence from analyses of surface soils and modern plants indicates that the relationship between the molecular distribution of long-chain n-alkanes of surface soils and source vegetation is highly complex,and is influenced by many factors.Further,it is suggested that source vegetation types should not be simply inferred from distribution patterns of long-chain n-alkanes in sediments.
