As an important intermediate product, short-chain fatty acids(SCFAs) can be generated after hydrolysis and acidification from waste activated sludge, and then can be transformed to methane during anaerobic digestion...As an important intermediate product, short-chain fatty acids(SCFAs) can be generated after hydrolysis and acidification from waste activated sludge, and then can be transformed to methane during anaerobic digestion process. In order to obtain more SCFA and methane,most studies in literatures were centered on enhancing the hydrolysis of sludge anaerobic digestion which was proved as un-efficient. Though the alkaline pretreatment in our previous study increased both the hydrolysis and acidification processes, it had a vast chemical cost which was considered uneconomical. In this paper, a low energy consumption pretreatment method, i.e. enhanced the whole three stages of the anaerobic fermentation processes at the same time, was reported, by which hydrolysis and acidification were both enhanced, and the SCFA and methane generation can be significantly improved with a small quantity of chemical input. Firstly, the effect of different pretreated temperatures and pretreatment time on sludge hydrolyzation was compared. It was found that sludge pretreated at 100°C for 60 min can achieve the maximal hydrolyzation. Further, effects of different initial p Hs on acidification of the thermal pretreated sludge were investigated and the highest SCFA was observed at initial p H 9.0with fermentation time of 6 d, the production of which was 348.63 mg COD/g VSS(6.8 times higher than the blank test) and the acetic acid was dominant acid. Then, the mechanisms for this new pretreatment significantly improving SCFA production were discussed. Finally,the effect of this low energy consumption pretreatment on methane generation was investigated.展开更多
Formic acid(FA) dehydrogenation has attracted a lot of attentions since it is a convenient method for H_2 production. In this work, we designed a self-supporting fuel cell system, in which H_2 from FA is supplied in...Formic acid(FA) dehydrogenation has attracted a lot of attentions since it is a convenient method for H_2 production. In this work, we designed a self-supporting fuel cell system, in which H_2 from FA is supplied into the fuel cell, and the exhaust heat from the fuel cell supported the FA dehydrogenation. In order to realize the system, we synthesized a highly active and selective homogeneous catalyst Ir Cp*Cl_2 bpym for FA dehydrogenation. The turnover frequency(TOF) of the catalyst for FA dehydrogenation is as high as7150 h^(-1)at 50°C, and is up to 144,000 h^(-1)at 90°C. The catalyst also shows excellent catalytic stability for FA dehydrogenation after several cycles of test. The conversion ratio of FA can achieve 93.2%, and no carbon monoxide is detected in the evolved gas. Therefore, the evolved gas could be applied in the proton exchange membrane fuel cell(PEMFC) directly. This is a potential technology for hydrogen storage and generation. The power density of the PEMFC driven by the evolved gas could approximate to that using pure hydrogen.展开更多
The real-time second harmonic generation was employed to investigate the[2+2]photodimerization of styrylquinoline(SQ) derivatives in Langmuir-Blodgett(LB) monolayers deposited from aqueous subphases with differen...The real-time second harmonic generation was employed to investigate the[2+2]photodimerization of styrylquinoline(SQ) derivatives in Langmuir-Blodgett(LB) monolayers deposited from aqueous subphases with different acidity.It was discovered that the photodimerization rate constant significantly decreased upon the addition of acid.The additional atomic force microscopy measurements revealed that surface morphologies were correlated to the photodimerization kinetics.These experimental results provide direct evidence for the topo-chemical mechanisms of[2+2]photodimerization in LB films.The current study demonstrates that the intermolecular interactions and aggregation structures play important roles in the photochemical properties at surfaces.展开更多
Clastic rock reservoirs in petroliferous basins are generally rich in feldspars. Feldspar dissolution has developed widely in clastic reservoirs, and the resulting secondary pores are crucial in deeply buried reservoi...Clastic rock reservoirs in petroliferous basins are generally rich in feldspars. Feldspar dissolution has developed widely in clastic reservoirs, and the resulting secondary pores are crucial in deeply buried reservoirs. Based on a study of the diagenesis of clastic reservoirs in the Bohai Bay Basin, Tarim Basin, and Pearl River Mouth Basin and physical and numerical simulation experiments of fluid-rock interactions, this paper proposed a successive formation model of secondary pores via feldspar dissolution in deeply buried clastic reservoirs, considering the global research progresses in feldspar dissolution in clastic rocks. Feldspar dissolution can occur from shallow open systems to deep-ultra deep closed systems in petroliferous basins, resulting in the successive formation of secondary pores at different diagenetic stages. The successive mechanism includes three aspects. The first aspect is the succession of corrosive fluids that dissolve minerals. Meteoric freshwater dominates at the Earth’s surface and the early diagenetic A stage. Subsequently, organic acids and COformed via kerogen maturation dominate at the early diagenetic B stage to the middle diagenetic stage. COand organic acids formed via hydrocarbon oxidation in hydrocarbon reservoirs dominate at the middle diagenetic B stage to the late diagenetic stage. The second aspect is the successive formation processes of secondary pores via feldspar dissolution. Large-scale feldspar secondary pores identified in deep reservoirs include secondary pores formed at shallow-medium depths that are subsequently preserved into deep layers, as well as secondary pores formed at deep depths. Existing secondary pores in deeply buried reservoirs are the superposition of successively feldspar dissolution caused by different acids at different stages. The third aspect is a successive change in the feldspar alteration pathways and porosity enhancement/preservation effect. Open to semi-open diagenetic systems are developed from the Earth’s surface to the early diagenetic stage, and feldspar dissolution forms enhanced secondary pores. Nearly closed to closed diagenetic systems develop in the middle to late diagenetic stages, and feldspar dissolution forms redistributional secondary pores. The associated cementation causes compression resistance of the rock, which is favorable for the preservation of secondary pores in deep layers. These new insights extend the formation window of secondary pores in petroliferous basins from the traditional acid-oil generation window to a high-temperature gas generation window after hydrocarbon charging. The proposed model explains the genesis of deep-ultra deep high-quality reservoirs with low-permeability, medium-porosity and dominating feldspar secondary pores, which is significant for hydrocarbon exploration in deep to ultra-deep layers.展开更多
基金supported by the National Science Foundation of China (Grant no. 51408419)the National Key Technology Research and Development Program of China (Grant nos. 2014BAL02B02-03 and 2014BAC29B01)the Key Program for International S&T Cooperation Projects of China (Grant no. 2012DFG91380)
文摘As an important intermediate product, short-chain fatty acids(SCFAs) can be generated after hydrolysis and acidification from waste activated sludge, and then can be transformed to methane during anaerobic digestion process. In order to obtain more SCFA and methane,most studies in literatures were centered on enhancing the hydrolysis of sludge anaerobic digestion which was proved as un-efficient. Though the alkaline pretreatment in our previous study increased both the hydrolysis and acidification processes, it had a vast chemical cost which was considered uneconomical. In this paper, a low energy consumption pretreatment method, i.e. enhanced the whole three stages of the anaerobic fermentation processes at the same time, was reported, by which hydrolysis and acidification were both enhanced, and the SCFA and methane generation can be significantly improved with a small quantity of chemical input. Firstly, the effect of different pretreated temperatures and pretreatment time on sludge hydrolyzation was compared. It was found that sludge pretreated at 100°C for 60 min can achieve the maximal hydrolyzation. Further, effects of different initial p Hs on acidification of the thermal pretreated sludge were investigated and the highest SCFA was observed at initial p H 9.0with fermentation time of 6 d, the production of which was 348.63 mg COD/g VSS(6.8 times higher than the blank test) and the acetic acid was dominant acid. Then, the mechanisms for this new pretreatment significantly improving SCFA production were discussed. Finally,the effect of this low energy consumption pretreatment on methane generation was investigated.
基金financial support granted by Ministry of Science and Technology of China(Nos.2016YFE0105700,2016YFA0200700)the National Natural Science Foundation of China(Nos.21373264,21573275)+2 种基金the Natural Science Foundation of Jiangsu Province(No.BK20150362)Suzhou Institute of Nano-tech and Nano-bionics(No.Y3AAA11004)Thousand Youth Talents Plan(No.Y3BQA11001)
文摘Formic acid(FA) dehydrogenation has attracted a lot of attentions since it is a convenient method for H_2 production. In this work, we designed a self-supporting fuel cell system, in which H_2 from FA is supplied into the fuel cell, and the exhaust heat from the fuel cell supported the FA dehydrogenation. In order to realize the system, we synthesized a highly active and selective homogeneous catalyst Ir Cp*Cl_2 bpym for FA dehydrogenation. The turnover frequency(TOF) of the catalyst for FA dehydrogenation is as high as7150 h^(-1)at 50°C, and is up to 144,000 h^(-1)at 90°C. The catalyst also shows excellent catalytic stability for FA dehydrogenation after several cycles of test. The conversion ratio of FA can achieve 93.2%, and no carbon monoxide is detected in the evolved gas. Therefore, the evolved gas could be applied in the proton exchange membrane fuel cell(PEMFC) directly. This is a potential technology for hydrogen storage and generation. The power density of the PEMFC driven by the evolved gas could approximate to that using pure hydrogen.
基金supported by the National Natural Science Foundation of China(Nos.21473217,21227802 and 21303216)the Chinese Ministry of Science and Technology(No.2013CB834504)
文摘The real-time second harmonic generation was employed to investigate the[2+2]photodimerization of styrylquinoline(SQ) derivatives in Langmuir-Blodgett(LB) monolayers deposited from aqueous subphases with different acidity.It was discovered that the photodimerization rate constant significantly decreased upon the addition of acid.The additional atomic force microscopy measurements revealed that surface morphologies were correlated to the photodimerization kinetics.These experimental results provide direct evidence for the topo-chemical mechanisms of[2+2]photodimerization in LB films.The current study demonstrates that the intermolecular interactions and aggregation structures play important roles in the photochemical properties at surfaces.
基金supported by the National Natural Science Foundation of China (Grant Nos. 41872140, 41821002, 41911530189)the National Major Science and Technology Special Grant (Grant No. 2016ZX05006-007)+2 种基金the Special Fund for Taishan Scholar Project (Grant No. tsqn201909061)the Fundamental Research Funds for the Central Universities (Grant No. 20CX06067A)the Marine S&T Fund of Shandong Province for Pilot National Laboratory for Marine Science and Technology (Qingdao) (Grant No. 2021QNLM020001)。
文摘Clastic rock reservoirs in petroliferous basins are generally rich in feldspars. Feldspar dissolution has developed widely in clastic reservoirs, and the resulting secondary pores are crucial in deeply buried reservoirs. Based on a study of the diagenesis of clastic reservoirs in the Bohai Bay Basin, Tarim Basin, and Pearl River Mouth Basin and physical and numerical simulation experiments of fluid-rock interactions, this paper proposed a successive formation model of secondary pores via feldspar dissolution in deeply buried clastic reservoirs, considering the global research progresses in feldspar dissolution in clastic rocks. Feldspar dissolution can occur from shallow open systems to deep-ultra deep closed systems in petroliferous basins, resulting in the successive formation of secondary pores at different diagenetic stages. The successive mechanism includes three aspects. The first aspect is the succession of corrosive fluids that dissolve minerals. Meteoric freshwater dominates at the Earth’s surface and the early diagenetic A stage. Subsequently, organic acids and COformed via kerogen maturation dominate at the early diagenetic B stage to the middle diagenetic stage. COand organic acids formed via hydrocarbon oxidation in hydrocarbon reservoirs dominate at the middle diagenetic B stage to the late diagenetic stage. The second aspect is the successive formation processes of secondary pores via feldspar dissolution. Large-scale feldspar secondary pores identified in deep reservoirs include secondary pores formed at shallow-medium depths that are subsequently preserved into deep layers, as well as secondary pores formed at deep depths. Existing secondary pores in deeply buried reservoirs are the superposition of successively feldspar dissolution caused by different acids at different stages. The third aspect is a successive change in the feldspar alteration pathways and porosity enhancement/preservation effect. Open to semi-open diagenetic systems are developed from the Earth’s surface to the early diagenetic stage, and feldspar dissolution forms enhanced secondary pores. Nearly closed to closed diagenetic systems develop in the middle to late diagenetic stages, and feldspar dissolution forms redistributional secondary pores. The associated cementation causes compression resistance of the rock, which is favorable for the preservation of secondary pores in deep layers. These new insights extend the formation window of secondary pores in petroliferous basins from the traditional acid-oil generation window to a high-temperature gas generation window after hydrocarbon charging. The proposed model explains the genesis of deep-ultra deep high-quality reservoirs with low-permeability, medium-porosity and dominating feldspar secondary pores, which is significant for hydrocarbon exploration in deep to ultra-deep layers.