Elevated CO_(2)(eCO_(2))and rice cultivars can strongly alter CH_(4)and N_(2)O emissions from paddy fields.However,detailed information on how their interaction affects greenhouse gas fluxes in the field is still lack...Elevated CO_(2)(eCO_(2))and rice cultivars can strongly alter CH_(4)and N_(2)O emissions from paddy fields.However,detailed information on how their interaction affects greenhouse gas fluxes in the field is still lacking.In this study,we investigated CH_(4)and N_(2)O emissions and rice growth under two contrasting rice cultivars(the strongly and weakly responsive cultivars)in response to eCO_(2),200μmol mol^(-1)higher than the ambient CO_(2)(aCO_(2)),in Chinese subtropical rice systems relying on a multi-year in-situ free-air CO_(2)enrichment platform from 2016 to 2018.The results showed that compared to aCO_(2),eCO_(2)increased rice yield by 7%-31%,while it decreased seasonal cumulative CH_(4)and N_(2)O emissions by 10%-59%and 33%-70%,respectively,regardless of rice cultivar.The decrease in CH_(4) emissions under eCO_(2)was possibly ascribed to the lower CH_(4)production potential(MPP)and the higher CH_(4)oxidation potential(MOP)correlated with the higher soil redox potential(Eh)and O_(2)concentration([O_(2)])in the surface soil.The mitigating effect of eCO_(2)on N_(2)O emissions was likely associated with the reduction of soil soluble N content.The strongly responsive cultivars had lower CH_(4)and N_(2)O emissions than the weakly re sponsive cultivars,and the main reason might be that the former induced higher soil Eh and[O_(2)]in the surface soil and had larger plant biomass and greater N uptake.The findings indicated that breeding strongly responsive cultivars with the potential for greater rice production and lower greenhouse gas emissions is an effective agricultural practice to ensure food security and environmental sustainability under future climate change scenarios.展开更多
At room temperature,the conversion of greenhouse gases into valuable chemicals using metal-free catalysts for dry reforming of methane(DRM) is quite promising and challenging.Herein,we developed a novel covalent organ...At room temperature,the conversion of greenhouse gases into valuable chemicals using metal-free catalysts for dry reforming of methane(DRM) is quite promising and challenging.Herein,we developed a novel covalent organic porous polymer (TPE-COP) with rapid charge separation of the electron–hole pairs for DRM driven by visible light at room temperature,which can efficiently generate syngas (CO and H_(2)).Both electron donor (tris(4-aminophenyl)amine,TAPA) and acceptor (4,4',4'',4'''-((1 E,1'E,1''E,1'''E)-(ethene-1,1,2,2-tetrayltetrakis (benzene-4,1-diyl))tetrakis (ethene-2,1-diyl))tetrakis (1-(4-formylbenzyl)quinolin-1-ium),TPE-CHO) were existed in TPE-COP,in which the push–pull effect between them promoted the separation of photogenerated electron–hole,thus greatly improving the photocatalytic activity.Density functional theory (DFT) simulation results show that TPE-COP can form charge-separating species under light irradiation,leading to electrons accumulation in TPE-CHO unit and holes in TAPA,and thus efficiently initiating DRM.After 20 h illumination,the photocatalytic results show that the yields reach 1123.6 and 30.8μmol g^(-1)for CO and H_(2),respectively,which are significantly higher than those of TPE-CHO small molecules.This excellent result is mainly due to the increase of specific surface area,the enhancement of light absorption capacity,and the improvement of photoelectron-generating efficiency after the formation of COP.Overall,this work contributes to understanding the advantages of COP materials for photocatalysis and fundamentally pushes metal-free catalysts into the door of DRM field.展开更多
High-solids anaerobic digestion of sewage sludge was a promising process, but high solid concentra- tion negatively influenced methane production. The influencing mechanism was systematically analyzed in this study th...High-solids anaerobic digestion of sewage sludge was a promising process, but high solid concentra- tion negatively influenced methane production. The influencing mechanism was systematically analyzed in this study through a series of static anaerobic digestion experiments at total solids （TS） contents of 3%--15%. The results showed that TS 6% was the boundary between low- solids and high-solids anaerobic digestion, and the accumulative methane yield decreased exponentially when TS increased from 6% to 15%. The performance of anaerobic digestion was directly determined by the efficiency of mass transfer, and the relation between methane yield and sludge diffusive coefficients was well described by a power function. Thus, the increasing TS resulted in an exponential increase in sludge viscosity but an exponential decrease in diffusive coefficient. The blocked mass transfer led to the accumulation of volatile fatty acids （VFAs） and free ammonia. Acetic metabolism was the main process, whereas butyric and propionic metabolisms occurred at the initial stage of high-solids anaerobic digestion. The concentration of VFAs reached the maximum at the initial stage, which were still lower than the threshold influencing methanogens. The concen- tration of free ammonia increased gradually, and the methanogenesis was inhibited when free ammonia nitro- gen exceeded 50 mg.L^-1. Consequently, the deterioration of high-solids anaerobic digestion was related to the blocked mass transfer and the resulting ammonia accumu- lation.展开更多
The infrared emission spectra of methane, H, CH and C2 hydrocarbons in natural gas were measured. The process of methane decomposition and C2 hydrocarbons formation was investigated. The experiment showed that the tim...The infrared emission spectra of methane, H, CH and C2 hydrocarbons in natural gas were measured. The process of methane decomposition and C2 hydrocarbons formation was investigated. The experiment showed that the time and conditions of methane decomposition and C2 hydrocarbons formation were different. Methane conversion rate increased with the increase in the current and decrease in the amount of methane. Furthermore, an examination of the reaction mechanisms revealed that free radicals played an important role in the chain reaction.展开更多
SA （sulfamic acid） catalyzes the reaction of indole with aldehyde and ketone to afford bis（indol-3-yl）methanes in good to excellent yields under solvent-free condition at ambient temperature.
K-Chabazite(K-CHA)zeolites were synthesized with an ultrafast procedure through an eco-friendly and cost-effective“one-pot”method.By solely employing colloidal silica and aluminum hydroxide in the K^(+)/Sr^(2+)syste...K-Chabazite(K-CHA)zeolites were synthesized with an ultrafast procedure through an eco-friendly and cost-effective“one-pot”method.By solely employing colloidal silica and aluminum hydroxide in the K^(+)/Sr^(2+)system without the assistance of seeds,fluorides or organic structure as directing agents,the K-CHA nano-aggregates were successfully synthesized in a few hours.The crystallization behavior of the gels with different SiO_(2)/Al_(2)O_(3) molar ratios(SARs)was investigated using X-ray diffraction(XRD);scanning electron microscope(SEM);X-ray fluorescence(XRF);27Al and 29Si magic angle spinning nuclear magnetic resonance(MAS NMR);Fourier-transform infrared spectra(FTIR);UV-Raman characterizations.As the nucleation rates were changed with the SARs,three kinds of K-CHA nano-aggregates,namely,hamburger-,disk-and walnut-shaped,were obtained.A possible formation mechanism of the K-CHA nano-aggregates was proposed.Additionally,the walnut-shaped sample with an SAR of 7 possessed the largest pore volume and specific surface area,resulting in the highest methane adsorption capacity.Furthermore,it exhibited a CH_(4)/N_(2) selectivity of more than 3 under relative pressures ranging from 0 to 0.6.This work offers guidance for modifying the stacking modes of other nano-sized zeolites.展开更多
基金supported by the National Key Research and Development Program of China(No.2017YFD0300105)the National Natural Science Foundation of China(No.41877325)the Youth Innovation Promotion Association of Chinese Academy of Sciences(No.2018349)。
文摘Elevated CO_(2)(eCO_(2))and rice cultivars can strongly alter CH_(4)and N_(2)O emissions from paddy fields.However,detailed information on how their interaction affects greenhouse gas fluxes in the field is still lacking.In this study,we investigated CH_(4)and N_(2)O emissions and rice growth under two contrasting rice cultivars(the strongly and weakly responsive cultivars)in response to eCO_(2),200μmol mol^(-1)higher than the ambient CO_(2)(aCO_(2)),in Chinese subtropical rice systems relying on a multi-year in-situ free-air CO_(2)enrichment platform from 2016 to 2018.The results showed that compared to aCO_(2),eCO_(2)increased rice yield by 7%-31%,while it decreased seasonal cumulative CH_(4)and N_(2)O emissions by 10%-59%and 33%-70%,respectively,regardless of rice cultivar.The decrease in CH_(4) emissions under eCO_(2)was possibly ascribed to the lower CH_(4)production potential(MPP)and the higher CH_(4)oxidation potential(MOP)correlated with the higher soil redox potential(Eh)and O_(2)concentration([O_(2)])in the surface soil.The mitigating effect of eCO_(2)on N_(2)O emissions was likely associated with the reduction of soil soluble N content.The strongly responsive cultivars had lower CH_(4)and N_(2)O emissions than the weakly re sponsive cultivars,and the main reason might be that the former induced higher soil Eh and[O_(2)]in the surface soil and had larger plant biomass and greater N uptake.The findings indicated that breeding strongly responsive cultivars with the potential for greater rice production and lower greenhouse gas emissions is an effective agricultural practice to ensure food security and environmental sustainability under future climate change scenarios.
基金supported by National Natural Science Foundation of China (Nos. 22274039 and 22178089)Hunan Provincial Innovation Foundation for Postgraduate (No.CX20220392)。
文摘At room temperature,the conversion of greenhouse gases into valuable chemicals using metal-free catalysts for dry reforming of methane(DRM) is quite promising and challenging.Herein,we developed a novel covalent organic porous polymer (TPE-COP) with rapid charge separation of the electron–hole pairs for DRM driven by visible light at room temperature,which can efficiently generate syngas (CO and H_(2)).Both electron donor (tris(4-aminophenyl)amine,TAPA) and acceptor (4,4',4'',4'''-((1 E,1'E,1''E,1'''E)-(ethene-1,1,2,2-tetrayltetrakis (benzene-4,1-diyl))tetrakis (ethene-2,1-diyl))tetrakis (1-(4-formylbenzyl)quinolin-1-ium),TPE-CHO) were existed in TPE-COP,in which the push–pull effect between them promoted the separation of photogenerated electron–hole,thus greatly improving the photocatalytic activity.Density functional theory (DFT) simulation results show that TPE-COP can form charge-separating species under light irradiation,leading to electrons accumulation in TPE-CHO unit and holes in TAPA,and thus efficiently initiating DRM.After 20 h illumination,the photocatalytic results show that the yields reach 1123.6 and 30.8μmol g^(-1)for CO and H_(2),respectively,which are significantly higher than those of TPE-CHO small molecules.This excellent result is mainly due to the increase of specific surface area,the enhancement of light absorption capacity,and the improvement of photoelectron-generating efficiency after the formation of COP.Overall,this work contributes to understanding the advantages of COP materials for photocatalysis and fundamentally pushes metal-free catalysts into the door of DRM field.
文摘High-solids anaerobic digestion of sewage sludge was a promising process, but high solid concentra- tion negatively influenced methane production. The influencing mechanism was systematically analyzed in this study through a series of static anaerobic digestion experiments at total solids （TS） contents of 3%--15%. The results showed that TS 6% was the boundary between low- solids and high-solids anaerobic digestion, and the accumulative methane yield decreased exponentially when TS increased from 6% to 15%. The performance of anaerobic digestion was directly determined by the efficiency of mass transfer, and the relation between methane yield and sludge diffusive coefficients was well described by a power function. Thus, the increasing TS resulted in an exponential increase in sludge viscosity but an exponential decrease in diffusive coefficient. The blocked mass transfer led to the accumulation of volatile fatty acids （VFAs） and free ammonia. Acetic metabolism was the main process, whereas butyric and propionic metabolisms occurred at the initial stage of high-solids anaerobic digestion. The concentration of VFAs reached the maximum at the initial stage, which were still lower than the threshold influencing methanogens. The concen- tration of free ammonia increased gradually, and the methanogenesis was inhibited when free ammonia nitro- gen exceeded 50 mg.L^-1. Consequently, the deterioration of high-solids anaerobic digestion was related to the blocked mass transfer and the resulting ammonia accumu- lation.
基金supported by National Natural Science Foundation of ChinaDoctoral Foundation of Ministry of Education(20010698007)Returned Scholars Foundation of Ministry of Education(2001[345])
文摘The infrared emission spectra of methane, H, CH and C2 hydrocarbons in natural gas were measured. The process of methane decomposition and C2 hydrocarbons formation was investigated. The experiment showed that the time and conditions of methane decomposition and C2 hydrocarbons formation were different. Methane conversion rate increased with the increase in the current and decrease in the amount of methane. Furthermore, an examination of the reaction mechanisms revealed that free radicals played an important role in the chain reaction.
文摘SA （sulfamic acid） catalyzes the reaction of indole with aldehyde and ketone to afford bis（indol-3-yl）methanes in good to excellent yields under solvent-free condition at ambient temperature.
基金supported by the National Natural Science Foundation of China(No.21276183).
文摘K-Chabazite(K-CHA)zeolites were synthesized with an ultrafast procedure through an eco-friendly and cost-effective“one-pot”method.By solely employing colloidal silica and aluminum hydroxide in the K^(+)/Sr^(2+)system without the assistance of seeds,fluorides or organic structure as directing agents,the K-CHA nano-aggregates were successfully synthesized in a few hours.The crystallization behavior of the gels with different SiO_(2)/Al_(2)O_(3) molar ratios(SARs)was investigated using X-ray diffraction(XRD);scanning electron microscope(SEM);X-ray fluorescence(XRF);27Al and 29Si magic angle spinning nuclear magnetic resonance(MAS NMR);Fourier-transform infrared spectra(FTIR);UV-Raman characterizations.As the nucleation rates were changed with the SARs,three kinds of K-CHA nano-aggregates,namely,hamburger-,disk-and walnut-shaped,were obtained.A possible formation mechanism of the K-CHA nano-aggregates was proposed.Additionally,the walnut-shaped sample with an SAR of 7 possessed the largest pore volume and specific surface area,resulting in the highest methane adsorption capacity.Furthermore,it exhibited a CH_(4)/N_(2) selectivity of more than 3 under relative pressures ranging from 0 to 0.6.This work offers guidance for modifying the stacking modes of other nano-sized zeolites.
