Currently,the solid adsorbents with porous structure have been widely applied in CO_(2)capture.However,the unmodified MgO-ZrO_(2)adsorbents appeared to be low adsorption capacity of CO_(2).The solid adsorbent material...Currently,the solid adsorbents with porous structure have been widely applied in CO_(2)capture.However,the unmodified MgO-ZrO_(2)adsorbents appeared to be low adsorption capacity of CO_(2).The solid adsorbent materials were successfully synthesized by loading TEPA onto the pore MgO/ZrO_(2)carriers in the paper.The pore structure and surface characteristic of the samples were analyzed by using XRD,BET,FT-IR and SEM.The adsorbent materials exhibited microcrystalline state,and the crystallinity of all samples gradually decreased as the increase of TEPA content.The pore structure analysis indicated that the modification of MgO-ZrO_(2)adsorbents with TEPA led to the decrease of the specific surface areas,but the narrow micro-mesopore size distributions ranging from 1.8-12 nm in the adsorbents still were maintained.FT-IR spectrum results further verified the successful loading of TEPA.The adsorption capacity of the adsorbents for CO_(2)were tested by using an adsorption apparatus equipped with gas chromatography.The results indicated that when the TEPA loading reached 50%,the sample exhibited the maximum adsorption value for CO_(2),reaching 4.07 mmol/g under the operation condition of 75℃and atmospheric pressure.This result could be assigned to not only the base active sites but also the coexistence of both micropore and mesopore in the adsorbent.After three cycles tests for CO_(2)capture,the adsorption value of the sample for CO_(2)can also reached 95%of its original adsorption capacity,which verified the excellent cyclic operation stability.展开更多
A series of amine-based adsorbents were synthesized using siliceous MCM-41 individually impregnated with four different amines（ethylenediamine（EDA）,diethylenetriamine（DETA）,tetraethylenepentamine（TEPA） and pent...A series of amine-based adsorbents were synthesized using siliceous MCM-41 individually impregnated with four different amines（ethylenediamine（EDA）,diethylenetriamine（DETA）,tetraethylenepentamine（TEPA） and pentaethylenehexamine（PEHA）） to study the effect of amine chain length and loading weight on their CO2 adsorption performances in detail.The adsorbents were characterized by FT-IR,elemental analysis,and thermo-gravimetric analysis to confirm their structure properties.Thermo-gravimetric analysis was also used to evaluate the CO2 adsorption performance of adsorbents.Longer chain amine-based materials can achieve higher amine loadings and show better thermal stability.The CO2 adsorption capacities at different temperatures indicate that the CO2 adsorption is thermodynamically controlled over EDAMCM41 and DETA-MCM41,while the adsorption over TEPA-MCM41 and PEHA-MCM41 is under kinetic control at low temperature.The chain length of amines affects the CO2 adsorption performance and the adsorption mechanism significantly.The results also indicate that CO2 adsorption capacity can be enhanced despite of high operation temperatures,if appropriate amines（TEPA and PEHA） are applied.However,adsorbents with short chain amine exhibit higher adsorption and desorption rates due to the collaborative effect of rapid reaction mechanisms of primary amines and less diffusion resistance of shorter chain length amines.展开更多
Chemoselective amine bioco njugation has long been a challenge for native protein modification.Inspired by Thiele’s seminal discovery,Li and co-workers recently developed an orto-phthalaldehyde(OPA)based reagent for ...Chemoselective amine bioco njugation has long been a challenge for native protein modification.Inspired by Thiele’s seminal discovery,Li and co-workers recently developed an orto-phthalaldehyde(OPA)based reagent for labeling the amino group of a protein.Here we report an expeditious and scalable synthesis of a Li-Thiele reagent featuring an arene construction strategy.The reagent contains an alkyne side chain as a handle for secondary modification.展开更多
In this work,shale hydration Inhibition performance of tallow amine ethoxylate as a shale stabilizer in water based drilling fluid,was investigated through these tests:bentonite hydration inhibition test,bentonite sed...In this work,shale hydration Inhibition performance of tallow amine ethoxylate as a shale stabilizer in water based drilling fluid,was investigated through these tests:bentonite hydration inhibition test,bentonite sedimentation test,drill cutting recovery test,dynamic linear swelling test,wettability test,isothermal water adsorption test,and zeta potential test.The results showed that bentonite particles are not capable of being hydrated or dispersed in the mediums containing tallow amine ethoxylate;tallow amine ethoxylate had shown a comparable and competitive inhibition performance with potassium chloride as a common shale stabilizer in drilling industry.Some amine functional groups exist in tallow amine ethoxylate structure which are capable of forming hydrogen bonding with surfaces of bentonite particles.This phenomenon decreased the water adsorption on bentonite particles'surfaces which results in reduction of swelling.Tallow amine ethoxylate is also compatible with other common drilling fluid additives.展开更多
A novel PdC12/bis（2-pyridylmethyl）amine-based ligand （1） catalytic system, which is water-soluble and air-stable, has been successfully synthesized and applied for Suzuki-Miyaura cross-coupling reaction. In the pr...A novel PdC12/bis（2-pyridylmethyl）amine-based ligand （1） catalytic system, which is water-soluble and air-stable, has been successfully synthesized and applied for Suzuki-Miyaura cross-coupling reaction. In the presence of catalytic amount of PdCl2/1 system, arylboronic acids can couple with a wide range of aryl halides, including aryl bromides and aryl chlorides. The reactions proceed under mild conditions to give excellent yields, and a wide range of functionalities is tolerated.展开更多
Chemical absorption with amine-based solvents was treated as a promising route approach for carbon dioxide(CO_(2))capture from industrial flue gases.The heat-stable salts(HSS)degraded from amine species is unavoidable...Chemical absorption with amine-based solvents was treated as a promising route approach for carbon dioxide(CO_(2))capture from industrial flue gases.The heat-stable salts(HSS)degraded from amine species is unavoidable and detrimental for CO_(2)capture.To solve this problem,17 porous materials,including anion-exchange resins,macroporous adsorption resins,and activated carbon,were selected for the purification of the hazardous HSS to regenerate the biphasic solvents.The purification performance was thoroughly assessed through experimental tests that examined the effects of various factors,including temperature,flow rate,and pH.Among the materials tested,the macroporous adsorption resin(NKA-9)demonstrated the highest purification efficiency,achieving an adsorption efficiency 92.0%for NO_(3)^(-),and an overall efficiency of 51%for HSS removal.The experimental tests showed that pH was the most significant factor.The decreasing pH value was detrimental to HSS purification.Additionally,a multi-step purification process combining anion exchange resin,activated carbon,and macroporous adsorption resin was evaluated.The multi-stage process effectively removes 82.98%HSS and 62.44%Fe^(3+)ions.The presented work holds significant importance for controlling the HSS concentration in amine-based solvent and maintaining the long-term efficient operation of CO_(2)capture process.展开更多
Due to the advantages of low energy consumption and high CO_(2) selectivity, the development of solid amine-based materials has been regarded as a hot research topic in the field of DAC for the past decades.The adsorp...Due to the advantages of low energy consumption and high CO_(2) selectivity, the development of solid amine-based materials has been regarded as a hot research topic in the field of DAC for the past decades.The adsorption capacity and stability over multiple cycles have been the top priorities for evaluation of practical application value. Herein, we synthesized a novel DAC material by loading TEPA onto defect-rich Mg_(0.55)Al-O MMOs with enhanced charge transfer effect. The optimal Mg_(0.55)Al-O-TEPA67% demonstrates the highest CO_(2)uptake of(3.0 mmol g^(-1)) and excellent regenerability, maintaining ~90% of the initial adsorption amount after 80 adsorption/desorption cycles. The in situ DRIFTS experiments suggested the formation of bicarbonate species under wet conditions. DFT calculations indicated that the stronger bonding between Mg_(0.55)Al-O support and solid amine was caused by the abundance of oxygen defects on MMOs confirmed by XPS and ESR, which favors the charge transfer between the support and amine,resulting in intense interaction and excellent regenerability. This work for the first time conducted comprehensive and systematic investigation on the stabilization mechanism for MMOs supported solid amine adsorbents with highest uptake and superior cyclic stability in depth, which is different from the most popular SiO_(2)-support, thus providing facile strategy and comprehensive theoretical mechanism support for future research about DAC materials.展开更多
基金supported by Shanxi Provincial Key Research and Development Project(202102090301026)Graduate Education Innovation Project of Taiyuan University of Science and Technology(SY2023024)。
文摘Currently,the solid adsorbents with porous structure have been widely applied in CO_(2)capture.However,the unmodified MgO-ZrO_(2)adsorbents appeared to be low adsorption capacity of CO_(2).The solid adsorbent materials were successfully synthesized by loading TEPA onto the pore MgO/ZrO_(2)carriers in the paper.The pore structure and surface characteristic of the samples were analyzed by using XRD,BET,FT-IR and SEM.The adsorbent materials exhibited microcrystalline state,and the crystallinity of all samples gradually decreased as the increase of TEPA content.The pore structure analysis indicated that the modification of MgO-ZrO_(2)adsorbents with TEPA led to the decrease of the specific surface areas,but the narrow micro-mesopore size distributions ranging from 1.8-12 nm in the adsorbents still were maintained.FT-IR spectrum results further verified the successful loading of TEPA.The adsorption capacity of the adsorbents for CO_(2)were tested by using an adsorption apparatus equipped with gas chromatography.The results indicated that when the TEPA loading reached 50%,the sample exhibited the maximum adsorption value for CO_(2),reaching 4.07 mmol/g under the operation condition of 75℃and atmospheric pressure.This result could be assigned to not only the base active sites but also the coexistence of both micropore and mesopore in the adsorbent.After three cycles tests for CO_(2)capture,the adsorption value of the sample for CO_(2)can also reached 95%of its original adsorption capacity,which verified the excellent cyclic operation stability.
基金supported by the National Natural Science Foundation of China(91434120)the Fundamental Research Funds for the Central Universities(2014ZD06),and the 111 Project(No.B12034)
文摘A series of amine-based adsorbents were synthesized using siliceous MCM-41 individually impregnated with four different amines（ethylenediamine（EDA）,diethylenetriamine（DETA）,tetraethylenepentamine（TEPA） and pentaethylenehexamine（PEHA）） to study the effect of amine chain length and loading weight on their CO2 adsorption performances in detail.The adsorbents were characterized by FT-IR,elemental analysis,and thermo-gravimetric analysis to confirm their structure properties.Thermo-gravimetric analysis was also used to evaluate the CO2 adsorption performance of adsorbents.Longer chain amine-based materials can achieve higher amine loadings and show better thermal stability.The CO2 adsorption capacities at different temperatures indicate that the CO2 adsorption is thermodynamically controlled over EDAMCM41 and DETA-MCM41,while the adsorption over TEPA-MCM41 and PEHA-MCM41 is under kinetic control at low temperature.The chain length of amines affects the CO2 adsorption performance and the adsorption mechanism significantly.The results also indicate that CO2 adsorption capacity can be enhanced despite of high operation temperatures,if appropriate amines（TEPA and PEHA） are applied.However,adsorbents with short chain amine exhibit higher adsorption and desorption rates due to the collaborative effect of rapid reaction mechanisms of primary amines and less diffusion resistance of shorter chain length amines.
基金supported by Ministry of Science and Technology (National Key Research and Development Program of China,No.2018YFA0901900)the National Natural Science Foundation of China (Nos.21931014,21525209, 21621002,21772225,and 21761142003)+4 种基金Chinese Academy of Sciences (Strategic Priority Research Program,No.XDB20000000International Partner Program,No.121731KYSB20190039Key Research Program of Frontier Sciences,No.QYZDB-SSW-SLH040)Science and Technology Commission of Shanghai Municipality (No.17XD1404600)K.C.Wong Education Foundation。
文摘Chemoselective amine bioco njugation has long been a challenge for native protein modification.Inspired by Thiele’s seminal discovery,Li and co-workers recently developed an orto-phthalaldehyde(OPA)based reagent for labeling the amino group of a protein.Here we report an expeditious and scalable synthesis of a Li-Thiele reagent featuring an arene construction strategy.The reagent contains an alkyne side chain as a handle for secondary modification.
基金The authors thank Petroleum University of Technology(PUT)MS-9201309National Iranian Drilling Company(NIDC)C-26588-115/1581 for their great laboratory supports.Interminable specific appreciation honorably goes to Dr.Mohammad Kamal Ghassem Alaskari,Miss Nemati,laboratory head of Pars Drilling Fluids(PDF)company and also Mr.Nourbakhsh,member of Kimyagaran Chemical Industries Company,for their unforgettable conscientiously assistance to supplying the materials。
文摘In this work,shale hydration Inhibition performance of tallow amine ethoxylate as a shale stabilizer in water based drilling fluid,was investigated through these tests:bentonite hydration inhibition test,bentonite sedimentation test,drill cutting recovery test,dynamic linear swelling test,wettability test,isothermal water adsorption test,and zeta potential test.The results showed that bentonite particles are not capable of being hydrated or dispersed in the mediums containing tallow amine ethoxylate;tallow amine ethoxylate had shown a comparable and competitive inhibition performance with potassium chloride as a common shale stabilizer in drilling industry.Some amine functional groups exist in tallow amine ethoxylate structure which are capable of forming hydrogen bonding with surfaces of bentonite particles.This phenomenon decreased the water adsorption on bentonite particles'surfaces which results in reduction of swelling.Tallow amine ethoxylate is also compatible with other common drilling fluid additives.
文摘A novel PdC12/bis（2-pyridylmethyl）amine-based ligand （1） catalytic system, which is water-soluble and air-stable, has been successfully synthesized and applied for Suzuki-Miyaura cross-coupling reaction. In the presence of catalytic amount of PdCl2/1 system, arylboronic acids can couple with a wide range of aryl halides, including aryl bromides and aryl chlorides. The reactions proceed under mild conditions to give excellent yields, and a wide range of functionalities is tolerated.
基金the National Key Research and Development Program of China(No.2023YFC3707004)the Liaoning Province Natural Science Foundation Project of China(No.2023-MS-321)+2 种基金the Liaoning Province International Cooperation Project,China(No.2023030491-JH2/107)the Tsinghua University Open Fund,China(No.KY-2024126)the Northeast Geological Science and Technology Innovation Center,China(Nos.QCJJ2023-46 and QCJJ2023-50).
文摘Chemical absorption with amine-based solvents was treated as a promising route approach for carbon dioxide(CO_(2))capture from industrial flue gases.The heat-stable salts(HSS)degraded from amine species is unavoidable and detrimental for CO_(2)capture.To solve this problem,17 porous materials,including anion-exchange resins,macroporous adsorption resins,and activated carbon,were selected for the purification of the hazardous HSS to regenerate the biphasic solvents.The purification performance was thoroughly assessed through experimental tests that examined the effects of various factors,including temperature,flow rate,and pH.Among the materials tested,the macroporous adsorption resin(NKA-9)demonstrated the highest purification efficiency,achieving an adsorption efficiency 92.0%for NO_(3)^(-),and an overall efficiency of 51%for HSS removal.The experimental tests showed that pH was the most significant factor.The decreasing pH value was detrimental to HSS purification.Additionally,a multi-step purification process combining anion exchange resin,activated carbon,and macroporous adsorption resin was evaluated.The multi-stage process effectively removes 82.98%HSS and 62.44%Fe^(3+)ions.The presented work holds significant importance for controlling the HSS concentration in amine-based solvent and maintaining the long-term efficient operation of CO_(2)capture process.
基金supported by the Fundamental Research Funds for the Central Universities (2019JQ03015)the National Natural Science Foundation of China (42075169, U1810209)the Beijing Municipal Education Commission through the Innovative Transdisciplinary Program “Ecological Restoration Engineering”。
文摘Due to the advantages of low energy consumption and high CO_(2) selectivity, the development of solid amine-based materials has been regarded as a hot research topic in the field of DAC for the past decades.The adsorption capacity and stability over multiple cycles have been the top priorities for evaluation of practical application value. Herein, we synthesized a novel DAC material by loading TEPA onto defect-rich Mg_(0.55)Al-O MMOs with enhanced charge transfer effect. The optimal Mg_(0.55)Al-O-TEPA67% demonstrates the highest CO_(2)uptake of(3.0 mmol g^(-1)) and excellent regenerability, maintaining ~90% of the initial adsorption amount after 80 adsorption/desorption cycles. The in situ DRIFTS experiments suggested the formation of bicarbonate species under wet conditions. DFT calculations indicated that the stronger bonding between Mg_(0.55)Al-O support and solid amine was caused by the abundance of oxygen defects on MMOs confirmed by XPS and ESR, which favors the charge transfer between the support and amine,resulting in intense interaction and excellent regenerability. This work for the first time conducted comprehensive and systematic investigation on the stabilization mechanism for MMOs supported solid amine adsorbents with highest uptake and superior cyclic stability in depth, which is different from the most popular SiO_(2)-support, thus providing facile strategy and comprehensive theoretical mechanism support for future research about DAC materials.
