The intramolecular O−H…πhydrogen bond has garnered significant research interest in recent decades.In this work,we utilized the infrared(IR)-vacuum-ultraviolet(VUV)nonresonant ionization detected IR spectroscopy(NRI...The intramolecular O−H…πhydrogen bond has garnered significant research interest in recent decades.In this work,we utilized the infrared(IR)-vacuum-ultraviolet(VUV)nonresonant ionization detected IR spectroscopy(NRID-IR)method to study the molecular structure of neutral and cationic 2-methylallyl alcohol(MAA,CH_(2)=C(CH_(3))−CH_(2)−OH).Density functional theory calculations revealed five stable neutral and three stable cationic MAA conformers,respectively.Two neutral MAA conformers are expected to have an O−H…πintramolecular hydrogen bond interaction,based on the structural characterization that the OH group is directed toward the C=C double bond.The IR spectra of both neutral(2700−3700 cm^(−1))and cationic MAA(2500−7200 cm^(−1))were measured,and the anharmonic IR spectra were calculated at the B3LYP-D3(BJ)/def2-TZVPP level.The OH stretching vibration frequency of neutral MAA was observed at 3656 cm−1,slightly lower than those of methanol and ethanol.In contrast,the OH stretching vibration of cationic MAA was red-shifted by about 140 cm^(−1)compared to neutral MAA.The interaction region indicator and natural bond orbital analysis suggest that the O−H…πinteraction in neutral MAA is weak,and may not play a major role in stabilizing the neutral MAA.展开更多
A resource recycling technique of hydrogen production from the catalytic degradation of organics in wastewater by aqueous phase reforming (APR) has been proposed. It is worthy of noting that this technique may be a po...A resource recycling technique of hydrogen production from the catalytic degradation of organics in wastewater by aqueous phase reforming (APR) has been proposed. It is worthy of noting that this technique may be a potential way for the purification of refractory and highly toxic organics in water for hydrogen production. Hazardous organics (such as phenol, aniline, nitrobenzene, tetrahydrofuran (THF), toluene, N,N-dimethylformamide (DMF) and cyclohexanol) in water could be completely de-graded into H2 and CO2 with high selectivity over Raney Ni, and Sn-modified Raney Ni (Sn-Raney-Ni) or Pd/C catalyst under mild conditions. The experimental results operated in tubular and autoclave reactors, indicated that the degradation degree of organics and H2 selectivity could reach 100% under the optimal reaction conditions. The Sn-Raney-Ni (Sn/Ni=0.06) and Pd/C catalysts show better catalytic performances than the Raney Ni catalyst for the degradation of organics in water into H2 and CO2 by the aqueous phase reforming process.展开更多
Transformation-temperature-hydrogen pressure phase diagram was constructed for a Nd15Fe79B6 alloy in order to estimate appropriate conditions for hydrogenation, disproportionation, desorption and recombination reacti...Transformation-temperature-hydrogen pressure phase diagram was constructed for a Nd15Fe79B6 alloy in order to estimate appropriate conditions for hydrogenation, disproportionation, desorption and recombination reaction （the HDDR）. Optimised recom- bination time （the highest coercivity） was found to be 10 rain. for 5 g samples processed at 740 ℃. Several HDDR processes were carried out at 30 kPa of hydrogen pressure at various temperatures. No correlation between magnetic propertiec and a direction of measurement was observed for the samples processed at 740 ℃. Remanence anisotropy was induced along an alignment direction when the temperature of the HDDR process was increased up to 800 ℃ and 850℃ for 〈100 gm and 100-160 p.m particles, respec- tively. Simultaneously, a small drop in coercivity was observed in the direction of alignment for 〈100 pm particles, but no for 100-160 grn particles. Furthermore, probably an ordered phase was found by TEM microstructure analysis in the bulk sample dis- proportionated at 850 ℃ under 150 kPa of hydrogen. Grains with antiphase domains were observed and corresponding electron dif- fraction patterns were resolved, likely indicating superlattice structures.展开更多
Transition metal nitride/carbide(TMN/C)have been actively explored as low-cost hydrogen evolution reaction(HER)electrocatalysts owing to their Pt-like physical and chemical properties.Unfortunately,pure TMN/C suffers ...Transition metal nitride/carbide(TMN/C)have been actively explored as low-cost hydrogen evolution reaction(HER)electrocatalysts owing to their Pt-like physical and chemical properties.Unfortunately,pure TMN/C suffers from strong hydrogen adsorption and lacks active centers for water dissociation.Herein,we developed a switchable WO_(3)-based in situ gas–solid reaction for preparing sophisticated Fe-N doped WC and Fe-C doped WN nanoarrays.Interestingly,the switch of codoping and phase can be effectively manipulated by regulating the amount of ferrocene.Resultant Fe-C-WN and Fe-N-WC exhibit robust electrocatalytic performance for HER in alkaline and acid electrolytes,respectively.The collective collaboration of morphological,phase and electronic effects are suggested to be responsible for the superior HER activity.The smallest|ΔGH*|value of Fe-NWC indicates preferable hydrogen-evolving kinetics on the Fe-N-WC surface for HER under acid condition,while Fe-C-WN is suggested to be beneficial to the adsorption and dissociation of H_(2)O for HER in alkaline electrolyte.展开更多
The Yaha Gas Condensate Field is the largest one discovered in China so far. In order to enhance the condensate recovery, gas recycling at 50 MPa has been implemented in Yaha field. Such high-pressure injection is ver...The Yaha Gas Condensate Field is the largest one discovered in China so far. In order to enhance the condensate recovery, gas recycling at 50 MPa has been implemented in Yaha field. Such high-pressure injection is very rare throughout the world. This paper offers the description of the geology and fluid phase behavior of Yaha field. The reservoir productivity and injectivity equa-tions, the optimal development and well patterns are presented. The follow-up investigation of the design implementation leads to the reasonable adjustment of the original development plan. The perforation principle and program of gas recycling for Yaha field are set up. The numerical simula-tion is used to predict the future production performance of gas recycling. Finally, a complete set of high-pressure gas recycling technology suite has been established. The field has come on-stream for one and a half year with condensate throughput of 590000 t in 2001, and fat profit returned. The success of high-pressure gas recycling in the Yaha field is of considerable importance from the theoretical and practical points of view and will considerably benefit the future development of other gas condensate fields in China.展开更多
基金gratefully acknowledge the Dalian Coherent Light Source(DCLS)for support and assistanceThis work was supported by the National Natural Science Foundation of China(No.22288201)+1 种基金the Chinese Academy of Sciences(GJJSTD20220001)the Innovation Program for Quantum Science and Technology(No.2021ZD0303305).
文摘The intramolecular O−H…πhydrogen bond has garnered significant research interest in recent decades.In this work,we utilized the infrared(IR)-vacuum-ultraviolet(VUV)nonresonant ionization detected IR spectroscopy(NRID-IR)method to study the molecular structure of neutral and cationic 2-methylallyl alcohol(MAA,CH_(2)=C(CH_(3))−CH_(2)−OH).Density functional theory calculations revealed five stable neutral and three stable cationic MAA conformers,respectively.Two neutral MAA conformers are expected to have an O−H…πintramolecular hydrogen bond interaction,based on the structural characterization that the OH group is directed toward the C=C double bond.The IR spectra of both neutral(2700−3700 cm^(−1))and cationic MAA(2500−7200 cm^(−1))were measured,and the anharmonic IR spectra were calculated at the B3LYP-D3(BJ)/def2-TZVPP level.The OH stretching vibration frequency of neutral MAA was observed at 3656 cm−1,slightly lower than those of methanol and ethanol.In contrast,the OH stretching vibration of cationic MAA was red-shifted by about 140 cm^(−1)compared to neutral MAA.The interaction region indicator and natural bond orbital analysis suggest that the O−H…πinteraction in neutral MAA is weak,and may not play a major role in stabilizing the neutral MAA.
基金the Program for New Century Excellent Talents in University (Grant No. NCET-04-0557)the Specialized Research Fund for the Doctoral Program of High Education (Grant No. SRFDP-20060337001)
文摘A resource recycling technique of hydrogen production from the catalytic degradation of organics in wastewater by aqueous phase reforming (APR) has been proposed. It is worthy of noting that this technique may be a potential way for the purification of refractory and highly toxic organics in water for hydrogen production. Hazardous organics (such as phenol, aniline, nitrobenzene, tetrahydrofuran (THF), toluene, N,N-dimethylformamide (DMF) and cyclohexanol) in water could be completely de-graded into H2 and CO2 with high selectivity over Raney Ni, and Sn-modified Raney Ni (Sn-Raney-Ni) or Pd/C catalyst under mild conditions. The experimental results operated in tubular and autoclave reactors, indicated that the degradation degree of organics and H2 selectivity could reach 100% under the optimal reaction conditions. The Sn-Raney-Ni (Sn/Ni=0.06) and Pd/C catalysts show better catalytic performances than the Raney Ni catalyst for the degradation of organics in water into H2 and CO2 by the aqueous phase reforming process.
基金Project supported by the National Centre for Research and Development(INNOTECH-K2/IN2/18/181960/NCBR/13)
文摘Transformation-temperature-hydrogen pressure phase diagram was constructed for a Nd15Fe79B6 alloy in order to estimate appropriate conditions for hydrogenation, disproportionation, desorption and recombination reaction （the HDDR）. Optimised recom- bination time （the highest coercivity） was found to be 10 rain. for 5 g samples processed at 740 ℃. Several HDDR processes were carried out at 30 kPa of hydrogen pressure at various temperatures. No correlation between magnetic propertiec and a direction of measurement was observed for the samples processed at 740 ℃. Remanence anisotropy was induced along an alignment direction when the temperature of the HDDR process was increased up to 800 ℃ and 850℃ for 〈100 gm and 100-160 p.m particles, respec- tively. Simultaneously, a small drop in coercivity was observed in the direction of alignment for 〈100 pm particles, but no for 100-160 grn particles. Furthermore, probably an ordered phase was found by TEM microstructure analysis in the bulk sample dis- proportionated at 850 ℃ under 150 kPa of hydrogen. Grains with antiphase domains were observed and corresponding electron dif- fraction patterns were resolved, likely indicating superlattice structures.
基金supported by Shandong Provincial Natural Science Foundation(No.ZR2019BB025)the National Natural Science Foundation of China(Nos.21976014 and U1930402)+1 种基金The Fundamental Research Funds for the Central Universities(FRFTP-20-11B and FRF-BR-20-02B)the generous computer time from TianHe2-JK Supercomputer Center。
文摘Transition metal nitride/carbide(TMN/C)have been actively explored as low-cost hydrogen evolution reaction(HER)electrocatalysts owing to their Pt-like physical and chemical properties.Unfortunately,pure TMN/C suffers from strong hydrogen adsorption and lacks active centers for water dissociation.Herein,we developed a switchable WO_(3)-based in situ gas–solid reaction for preparing sophisticated Fe-N doped WC and Fe-C doped WN nanoarrays.Interestingly,the switch of codoping and phase can be effectively manipulated by regulating the amount of ferrocene.Resultant Fe-C-WN and Fe-N-WC exhibit robust electrocatalytic performance for HER in alkaline and acid electrolytes,respectively.The collective collaboration of morphological,phase and electronic effects are suggested to be responsible for the superior HER activity.The smallest|ΔGH*|value of Fe-NWC indicates preferable hydrogen-evolving kinetics on the Fe-N-WC surface for HER under acid condition,while Fe-C-WN is suggested to be beneficial to the adsorption and dissociation of H_(2)O for HER in alkaline electrolyte.
基金This work was supported by the Tenth Five-year Key Technologies R&D Programme (Grant No. 2001BA605A02)
文摘The Yaha Gas Condensate Field is the largest one discovered in China so far. In order to enhance the condensate recovery, gas recycling at 50 MPa has been implemented in Yaha field. Such high-pressure injection is very rare throughout the world. This paper offers the description of the geology and fluid phase behavior of Yaha field. The reservoir productivity and injectivity equa-tions, the optimal development and well patterns are presented. The follow-up investigation of the design implementation leads to the reasonable adjustment of the original development plan. The perforation principle and program of gas recycling for Yaha field are set up. The numerical simula-tion is used to predict the future production performance of gas recycling. Finally, a complete set of high-pressure gas recycling technology suite has been established. The field has come on-stream for one and a half year with condensate throughput of 590000 t in 2001, and fat profit returned. The success of high-pressure gas recycling in the Yaha field is of considerable importance from the theoretical and practical points of view and will considerably benefit the future development of other gas condensate fields in China.
