Alkane coupling with CO_(2) by metal-containing zeolites catalysis is found to be a promising way to produce aromatics and syngas in recent years,but the real active sites and the role of CO_(2) are still unclear owin...Alkane coupling with CO_(2) by metal-containing zeolites catalysis is found to be a promising way to produce aromatics and syngas in recent years,but the real active sites and the role of CO_(2) are still unclear owing to the quick evolution of the metallic active sites and the complex reaction processes including direct propane aromatization,CO_(2) hydrogenation,reverse water-gas shift reaction,and propane-CO_(2) coupling aromatization.Herein,Ga/ZSM-5 catalysts were constructed to study the dynamic evolution of the metallic active sites and the role of CO_(2) during the propane and CO_(2) coupling reaction.After optimizing the reaction conditions,a notable propane conversion rate of 97.9%and an impressive aromatics selectivity of 80.6%in hydrocarbons can be achieved at the conditions of 550℃and CO_(2)/C_(3)H_(8) of 4.^(13)CO_(2)isotope experiments illustrate that C-atoms of CO_(2) can enter into CO(86.5%)and aromatics(10.8%)during the propane-CO_(2) coupling reaction process.In situ XANES and FTIR spectroscopies at 550℃and H_(2)/C_(3)H_(8) atmosphere reveal that GaO_(x) species can be gradually dispersed into[GaH_(2)]^(+)/[GaH]^(2+)on the Bronsted acid sites of ZSM-5 zeolite during H_(2) and/or C_(3)H_(8) treatment,which are the real active sites for propane-CO_(2) coupling conversion.In situ CO_(2)-FTIR experiments demonstrate that the[GaH_(2)]^(+)/[GaH]^(2+)species can react with CO_(2) and accelerate the propane and CO_(2) coupling process.This work not only presents a cost-effective avenue for CO_(2) utilization,but also contributes to the active site design for improved alkane and CO_(2) activation in coupling reaction system.展开更多
Propane dehydrogenation(PDH)on Ga/H-ZSM-5 catalysts is a promising reaction for propylene production,while the detail mechanism remains debatable.Ga_(2)O_(2)^(2+) stabilized by framework Al pairs have been identified ...Propane dehydrogenation(PDH)on Ga/H-ZSM-5 catalysts is a promising reaction for propylene production,while the detail mechanism remains debatable.Ga_(2)O_(2)^(2+) stabilized by framework Al pairs have been identified as the most active species in Ga/H-ZSM-5 for PDH in our recent work.Here we demonstrate a strong correlation between the PDH activity and a fraction of Ga_(2)O_(2)^(2+) species corresponding to the infrared GaH band of higher wavenumber(GaHHW)in reduced Ga/H-ZSM-5,instead of the overall Ga_(2)O_(2)^(2+) species,by employing five H-ZSM-5 supports sourced differently with comparable Si/Al ratio.This disparity in Ga_(2)O_(2)^(2+) species stems from their differing capacity in completing the catalytic cycle.Spectroscopic results suggest that PDH proceeds via a two-step mechanism:(1)C-H bond activation of propane on H-Ga_(2)O_(2)^(2+) species(rate determining step);(2)β-hydride elimination of adsorbed propyl group,which only occurs on active Ga_(2)O_(2)^(2+) species corresponding to GaHHW.展开更多
Microplastics can influence global climate change by regulating the emissions of greenhouse gases from different ecosystems. The effects of microplastics in terrestrial ecosystems are still not well studied particular...Microplastics can influence global climate change by regulating the emissions of greenhouse gases from different ecosystems. The effects of microplastics in terrestrial ecosystems are still not well studied particularly greenhouse gases emissions. Thus, we conducted a laboratory experiment over a period of 90 days with two types of microplastics (differing in their chemical structure), high density polyethylene (HDPE) and low density polyethylene (LDPE), which were applied to the soil at a rate of 0% to 0.1% (w/w). The overarching aim was to investigate the effects of microplastic type, microplastic concentration and days of exposure on greenhouse gases emissions. We also used original and artificially weathered microplastics (the same HDPE and LDPE) to make a comparison of greenhouse gases emissions between the original microplastics treated soils and the soils treated with weathered microplastics. Our findings showed that HDPE and LDPE microplastics significantly increased the emissions of greenhouse gases from the soil than that of the control soils. Emissions were increased with the increases in the level of microplastic in the soil. The weathered microplastic emitted greater quantity of greenhouse gases compared to that of the original microplastics. In contrast to a low initial emission quantity, the emissions were gradually increased at the termination of the experiment. Our experiment on the emissions of greenhouse gases from the soil vis-à-vis microplastic additions indicated that the microplastic increased the emissions of greenhouse gases in terrestrial ecosystems, and pervasive microplastic impacts may have consequences for the global climate change. Greenhouse gases emissions from the soil not only depend on the type and concentration of the microplastic, but also on the days of exposure to the microplastic.展开更多
Deep oil and gas refer to oil and gas resources buried at a significant depth below the surface. Compared with conventional oil and gas, deep oil and gas often face more complex geological conditions and technological...Deep oil and gas refer to oil and gas resources buried at a significant depth below the surface. Compared with conventional oil and gas, deep oil and gas often face more complex geological conditions and technological challenges, therefore, the development and exploitation of these oil and gas resources require advanced technology and equipment. Use bibliometrics to study academic literature. Select available data and download it in “RefWorks” format. Import the data into Cite Space 6.3.R2 software for author collaboration and keyword emergence analysis and visualization. Use Microsoft Excel 2016 software to analyze the annual publication volume, literature institutions, and disciplinary distribution of domestic and international scholarly literature. Research has found that: 1) The institution with the highest number of publications in the field of deep oil and gas in China is the China Petroleum Exploration and Development Research Institute;The author with the highest number of publications is Zhu Guangyou;The author with the highest citation frequency is Jia Chengzao;The research work in the field of deep oil and gas in China is mainly led by national level fund projects. 2) The research hot-spots of deep oil and gas in China are showing a trend of shifting from Jilin and Henan to Xinjiang and Sichuan. 3) The research on deep oil and gas fields in the Paleogene of China is mainly concentrated in Henan Province and Shandong Province. The Lower Tertiary, Cambrian and Jurassic are respectively concentrated in Dongpu Sag, Dongying Sag, Sichuan Basin, Tarim Basin in Xinjiang, the Junggar Basin and Qaidam Basin in Qinghai. The Sinian, Ordovician, Cretaceous, and Neogene systems are mainly concentrated in Sichuan, Xinjiang, and Qinghai provinces. The Permian system is mainly located in the southwest and Northwest of China. This article uses a new research perspective and methodology to systematically analyze the current situation and future development trends of deep oil and gas exploration and development in China, which is of great significance for promoting effective exploration and development of deep oil and gas resources.展开更多
基金supported by the National Key Research and Development Program of China (No.2022YFE0116000)the National Natural Science Foundation of China (No.22288101,21991092,21991090,22202193,and 22172166)+1 种基金the Youth Innovation Promotion Association CAS (2021182)the Innovation Research Foundation of Dalian Institute of Chemical Physics,Chinese Academy of Sciences (DICP I202429 and I202217)。
文摘Alkane coupling with CO_(2) by metal-containing zeolites catalysis is found to be a promising way to produce aromatics and syngas in recent years,but the real active sites and the role of CO_(2) are still unclear owing to the quick evolution of the metallic active sites and the complex reaction processes including direct propane aromatization,CO_(2) hydrogenation,reverse water-gas shift reaction,and propane-CO_(2) coupling aromatization.Herein,Ga/ZSM-5 catalysts were constructed to study the dynamic evolution of the metallic active sites and the role of CO_(2) during the propane and CO_(2) coupling reaction.After optimizing the reaction conditions,a notable propane conversion rate of 97.9%and an impressive aromatics selectivity of 80.6%in hydrocarbons can be achieved at the conditions of 550℃and CO_(2)/C_(3)H_(8) of 4.^(13)CO_(2)isotope experiments illustrate that C-atoms of CO_(2) can enter into CO(86.5%)and aromatics(10.8%)during the propane-CO_(2) coupling reaction process.In situ XANES and FTIR spectroscopies at 550℃and H_(2)/C_(3)H_(8) atmosphere reveal that GaO_(x) species can be gradually dispersed into[GaH_(2)]^(+)/[GaH]^(2+)on the Bronsted acid sites of ZSM-5 zeolite during H_(2) and/or C_(3)H_(8) treatment,which are the real active sites for propane-CO_(2) coupling conversion.In situ CO_(2)-FTIR experiments demonstrate that the[GaH_(2)]^(+)/[GaH]^(2+)species can react with CO_(2) and accelerate the propane and CO_(2) coupling process.This work not only presents a cost-effective avenue for CO_(2) utilization,but also contributes to the active site design for improved alkane and CO_(2) activation in coupling reaction system.
文摘Propane dehydrogenation(PDH)on Ga/H-ZSM-5 catalysts is a promising reaction for propylene production,while the detail mechanism remains debatable.Ga_(2)O_(2)^(2+) stabilized by framework Al pairs have been identified as the most active species in Ga/H-ZSM-5 for PDH in our recent work.Here we demonstrate a strong correlation between the PDH activity and a fraction of Ga_(2)O_(2)^(2+) species corresponding to the infrared GaH band of higher wavenumber(GaHHW)in reduced Ga/H-ZSM-5,instead of the overall Ga_(2)O_(2)^(2+) species,by employing five H-ZSM-5 supports sourced differently with comparable Si/Al ratio.This disparity in Ga_(2)O_(2)^(2+) species stems from their differing capacity in completing the catalytic cycle.Spectroscopic results suggest that PDH proceeds via a two-step mechanism:(1)C-H bond activation of propane on H-Ga_(2)O_(2)^(2+) species(rate determining step);(2)β-hydride elimination of adsorbed propyl group,which only occurs on active Ga_(2)O_(2)^(2+) species corresponding to GaHHW.
文摘Microplastics can influence global climate change by regulating the emissions of greenhouse gases from different ecosystems. The effects of microplastics in terrestrial ecosystems are still not well studied particularly greenhouse gases emissions. Thus, we conducted a laboratory experiment over a period of 90 days with two types of microplastics (differing in their chemical structure), high density polyethylene (HDPE) and low density polyethylene (LDPE), which were applied to the soil at a rate of 0% to 0.1% (w/w). The overarching aim was to investigate the effects of microplastic type, microplastic concentration and days of exposure on greenhouse gases emissions. We also used original and artificially weathered microplastics (the same HDPE and LDPE) to make a comparison of greenhouse gases emissions between the original microplastics treated soils and the soils treated with weathered microplastics. Our findings showed that HDPE and LDPE microplastics significantly increased the emissions of greenhouse gases from the soil than that of the control soils. Emissions were increased with the increases in the level of microplastic in the soil. The weathered microplastic emitted greater quantity of greenhouse gases compared to that of the original microplastics. In contrast to a low initial emission quantity, the emissions were gradually increased at the termination of the experiment. Our experiment on the emissions of greenhouse gases from the soil vis-à-vis microplastic additions indicated that the microplastic increased the emissions of greenhouse gases in terrestrial ecosystems, and pervasive microplastic impacts may have consequences for the global climate change. Greenhouse gases emissions from the soil not only depend on the type and concentration of the microplastic, but also on the days of exposure to the microplastic.
文摘Deep oil and gas refer to oil and gas resources buried at a significant depth below the surface. Compared with conventional oil and gas, deep oil and gas often face more complex geological conditions and technological challenges, therefore, the development and exploitation of these oil and gas resources require advanced technology and equipment. Use bibliometrics to study academic literature. Select available data and download it in “RefWorks” format. Import the data into Cite Space 6.3.R2 software for author collaboration and keyword emergence analysis and visualization. Use Microsoft Excel 2016 software to analyze the annual publication volume, literature institutions, and disciplinary distribution of domestic and international scholarly literature. Research has found that: 1) The institution with the highest number of publications in the field of deep oil and gas in China is the China Petroleum Exploration and Development Research Institute;The author with the highest number of publications is Zhu Guangyou;The author with the highest citation frequency is Jia Chengzao;The research work in the field of deep oil and gas in China is mainly led by national level fund projects. 2) The research hot-spots of deep oil and gas in China are showing a trend of shifting from Jilin and Henan to Xinjiang and Sichuan. 3) The research on deep oil and gas fields in the Paleogene of China is mainly concentrated in Henan Province and Shandong Province. The Lower Tertiary, Cambrian and Jurassic are respectively concentrated in Dongpu Sag, Dongying Sag, Sichuan Basin, Tarim Basin in Xinjiang, the Junggar Basin and Qaidam Basin in Qinghai. The Sinian, Ordovician, Cretaceous, and Neogene systems are mainly concentrated in Sichuan, Xinjiang, and Qinghai provinces. The Permian system is mainly located in the southwest and Northwest of China. This article uses a new research perspective and methodology to systematically analyze the current situation and future development trends of deep oil and gas exploration and development in China, which is of great significance for promoting effective exploration and development of deep oil and gas resources.
