Background: Soil organic carbon(SOC) is a large reservoir of terrestrial carbon(C); it consists of different fractions of varying complexity and stability. Partitioning SOC into different pools of decomposability help...Background: Soil organic carbon(SOC) is a large reservoir of terrestrial carbon(C); it consists of different fractions of varying complexity and stability. Partitioning SOC into different pools of decomposability help better predict the trend of changes in SOC dynamics under climate change. Information on how physical fractions and chemical structures of SOC are related to climate and vegetation types is essential for spatial model ing of SOC processes and responses to global change factors.Method: Soil samples were col ected from multiple representative forest sites of three contrasting climatic zones(i.e. cool temperate, warm temperate, and subtropical) in eastern China. Measurements were made on SOC contents and physical fractions of the 0–20 cm soil layer, and the chemical composition of SOC of the 0–5 cm soil layer, along with measurements and compilation of the basic site and forest stand variables. The long-term effects of temperature, litter inputs, soil characteristics and vegetation type on the SOC contents and factions were examined by means of "space for time substitution" approach and statistical analysis.Result: Mean annual temperature(MAT) varied from 2.1 °C at the cool temperate sites to 20.8 °C at the subtropical sites. Total SOC of the 0–20 cm soil layer decreased with increasing MAT, ranging from 89.2 g·kg^(-1) in cool temperate forests to 57.7 g·kg^(-1) in subtropical forests, at an average rate of 1.87% reduction in SOC with a 1 °C increase in MAT.With increasing MAT, the proportions of aromatic C and phenolic C displayed a tendency of decreases, whereas the proportion of alkyl C and A/O-A value(the ratio of alkyl C to the sum of O-alkyl C and acetal C) displayed a tendency of increases. Overall, there were no significant changes with MAT and forest type in either the physical fractions or the chemical composition. Based on the relationship between the SOC content and MAT, we estimate that SOC in the top 20 soil layer of forests potentially contribute 6.58–26.3 Pg C globally to the atmosphere if global MAT increases by 1 °C–4 °C by the end of the twenty-first century, with nearly half of which(cf. 2.87–11.5 Pg C) occurring in the 0–5 cm mineral soils.Conclusion: Forest topsoil SOC content decreased and became chemical y more recalcitrant with increasing MAT,without apparent changes in the physical fractions of SOC.展开更多
The co-aromatization of methane with higher hydrocarbons represents a promising route to valorize methane, an abundant but underexploited carbon resource. In this study, we elucidate a novel approach to enhance the ca...The co-aromatization of methane with higher hydrocarbons represents a promising route to valorize methane, an abundant but underexploited carbon resource. In this study, we elucidate a novel approach to enhance the catalytic co-aromatization of hexane and methane by confining Pt within zeolite catalysts and modulating its electron density. Our findings show that encapsulating Pt within MFI structure is pivotal for activating the feedstock and fostering the formation of aromatic products. Interaction between K atoms and the silanol nest forms siloxy groups which are critical for the stabilization of Pt species. Tuning the K content in PtSn@MFI catalysts adeptly alters the electronic configuration of Pt clusters. This modification is corroborated by infrared and X-ray photoelectron spectroscopy analysis, and density functional theory calculations. Remarkably, the catalyst with 0.8 wt% K exhibits an optimal Pt electron density, driving its superior efficacy in the co-aromatization reaction, converting 0.78 mol of methane for each mole of hexane processed. By employing ~(13)C isotopic labeling and solid-state NMR studies, we demonstrate the participation of methane in the adsorbed species inside the zeolite channel and its incorporation to the benzyl site of the substitute group and phenyl rings in aromatic compounds, underscoring the importance of Pt encapsulation.展开更多
基金supported by the National Natural Science Foundation of China(Grant No.31470623)the National Basic Research Program of China(Grant No.2011CB403205)
文摘Background: Soil organic carbon(SOC) is a large reservoir of terrestrial carbon(C); it consists of different fractions of varying complexity and stability. Partitioning SOC into different pools of decomposability help better predict the trend of changes in SOC dynamics under climate change. Information on how physical fractions and chemical structures of SOC are related to climate and vegetation types is essential for spatial model ing of SOC processes and responses to global change factors.Method: Soil samples were col ected from multiple representative forest sites of three contrasting climatic zones(i.e. cool temperate, warm temperate, and subtropical) in eastern China. Measurements were made on SOC contents and physical fractions of the 0–20 cm soil layer, and the chemical composition of SOC of the 0–5 cm soil layer, along with measurements and compilation of the basic site and forest stand variables. The long-term effects of temperature, litter inputs, soil characteristics and vegetation type on the SOC contents and factions were examined by means of "space for time substitution" approach and statistical analysis.Result: Mean annual temperature(MAT) varied from 2.1 °C at the cool temperate sites to 20.8 °C at the subtropical sites. Total SOC of the 0–20 cm soil layer decreased with increasing MAT, ranging from 89.2 g·kg^(-1) in cool temperate forests to 57.7 g·kg^(-1) in subtropical forests, at an average rate of 1.87% reduction in SOC with a 1 °C increase in MAT.With increasing MAT, the proportions of aromatic C and phenolic C displayed a tendency of decreases, whereas the proportion of alkyl C and A/O-A value(the ratio of alkyl C to the sum of O-alkyl C and acetal C) displayed a tendency of increases. Overall, there were no significant changes with MAT and forest type in either the physical fractions or the chemical composition. Based on the relationship between the SOC content and MAT, we estimate that SOC in the top 20 soil layer of forests potentially contribute 6.58–26.3 Pg C globally to the atmosphere if global MAT increases by 1 °C–4 °C by the end of the twenty-first century, with nearly half of which(cf. 2.87–11.5 Pg C) occurring in the 0–5 cm mineral soils.Conclusion: Forest topsoil SOC content decreased and became chemical y more recalcitrant with increasing MAT,without apparent changes in the physical fractions of SOC.
基金supported by the National Natural Science Foundation of China(22002179)the Shanxi Provincial Science and Technology Department(YDZJSX2022A074)。
文摘The co-aromatization of methane with higher hydrocarbons represents a promising route to valorize methane, an abundant but underexploited carbon resource. In this study, we elucidate a novel approach to enhance the catalytic co-aromatization of hexane and methane by confining Pt within zeolite catalysts and modulating its electron density. Our findings show that encapsulating Pt within MFI structure is pivotal for activating the feedstock and fostering the formation of aromatic products. Interaction between K atoms and the silanol nest forms siloxy groups which are critical for the stabilization of Pt species. Tuning the K content in PtSn@MFI catalysts adeptly alters the electronic configuration of Pt clusters. This modification is corroborated by infrared and X-ray photoelectron spectroscopy analysis, and density functional theory calculations. Remarkably, the catalyst with 0.8 wt% K exhibits an optimal Pt electron density, driving its superior efficacy in the co-aromatization reaction, converting 0.78 mol of methane for each mole of hexane processed. By employing ~(13)C isotopic labeling and solid-state NMR studies, we demonstrate the participation of methane in the adsorbed species inside the zeolite channel and its incorporation to the benzyl site of the substitute group and phenyl rings in aromatic compounds, underscoring the importance of Pt encapsulation.
