Organic electrode materials are desirable for green and sustainable Li-ion batteries(LIBs) due to their light-weight, low cost, abundance and multi-electron transfer reactions during battery operation. However, the su...Organic electrode materials are desirable for green and sustainable Li-ion batteries(LIBs) due to their light-weight, low cost, abundance and multi-electron transfer reactions during battery operation. However, the successful utilization of organic electrodes is hindered by their poor electrical conductivity and low cyclic stability. Herein, a facile synthesis of π-conjugated N-containing heteroaromatic hexacarboxylate(Li6-HAT) compound and its electrochemical performance as an anode material in LIBs is reported.The as-synthesized Li6-HAT electrode renders an ultrahigh initial capacity of 1126.3 m Ah g^(-1) at the current density of 100 m A g^(-1). Moreover, π-conjugated N-containing heteroaromatic center provide excellent reversibility of(de)lithiation process, resulting in excellent capacity retention. Furthermore, a combination of density functional theory(DFT) calculations, in-situ Fourier transform infrared(FTIR) and ex-situ X-ray photoelectron spectroscopy(XPS) characterization reveal that the π-conjugated nitrogen and carboxyl oxygen act as electrochemically active sites during the charge/discharge process. The current work provides novel insights into the charge storage mechanism of organic electrodes and opens up avenues for further development and utilization of organic electrodes in Li-ion batteries.展开更多
A novel inorganic-organic hybrid borate,[Al2（fum）（H3BO3）（OH） 4]n·n（H3BO3） （1,H2fum = fumaric acid） ,has been synthesized and characterized by single-crystal X-ray diffraction,FTIR and elemental analysis...A novel inorganic-organic hybrid borate,[Al2（fum）（H3BO3）（OH） 4]n·n（H3BO3） （1,H2fum = fumaric acid） ,has been synthesized and characterized by single-crystal X-ray diffraction,FTIR and elemental analysis. Crystal data for compound 1： orthorhombic,space group Pnma,a = 14.108（3） ,b = 6.9412（14） ,c = 14.995（3）A,V = 1468.3（5）A^3,Z = 4,Mr = 359.72,Dc = 1.627 g/cm^3,μ = 0.254 mm^-1,F（000） = 736,the final R = 0.0492 and wR = 0.1650 with I 〉 2σ（I） . In compound 1,each Al^Ⅲ ion is coordinated by six oxygen atoms to adopt a distorted octahedral geometry. Both fumarate anion and the coordinated boric acid act as bidentate bridging ligands to link two neighboring Al^Ⅲ centers simultaneously. Each Al^Ⅲ ion is bridged by two μ2-hydroxyl ligands to construct an infinite wave-like [Al2（fum）（H3BO3）（OH） 4]n chain. These one-dimensional chains form hydrogen bonds with free boric acid molecules giving rise to a three-dimensional supramolecular network.展开更多
A series of thermoreversible konjac glucomannan gels crosslinked by organic borate were prepared. Required amount of hydrophilic SiO2 was added into the konjac glucomannan solutions before the crosslinking reaction, T...A series of thermoreversible konjac glucomannan gels crosslinked by organic borate were prepared. Required amount of hydrophilic SiO2 was added into the konjac glucomannan solutions before the crosslinking reaction, The gel network was formed through the crosslinking reaction between borate ions dissociated from organic borate and the cis-diol hydroxyl groups on the mannose units of polysaccharide chains. The rheological properties of the complex gels were studied by dynamic viscoelastic measurement. The gelation kinetics of the complex gels was studied and the critical getation points of the gels were exactly determined by the Winter-Chambon criterion. The effects of temperature and composite ratio on the shear storage modulus （G＇）, the loss modulus （G＂） and the sol-gel transition points were investigated.展开更多
A polyoxovanadium borate [Na（H2O）]2[Na（H2O）2]2[Cu（en）2][V12B18O54（OH）6]·（H3O）2·（H2O）18 1（en = ethylenediamine） has been hydrothermally synthesized and characterized by IR,two-dimensional infra...A polyoxovanadium borate [Na（H2O）]2[Na（H2O）2]2[Cu（en）2][V12B18O54（OH）6]·（H3O）2·（H2O）18 1（en = ethylenediamine） has been hydrothermally synthesized and characterized by IR,two-dimensional infrared（2D IR） correlation spectroscopy with magnetic and thermal perturba-tion,thermal IR spectroscopy,thermal gravimetric analysis and single-crystal X-ray diffraction.It crystallizes in triclinic,space group P with a = 12.981（3）,b = 13.044（3）,c = 14.208（3） ,α = 63.98（3）,β = 77.17（3）,γ = 14.208（3）°,V = 2001.0（8） 3,Z = 1,Mr = 2518.05,Dc = 2.090 g/cm-1,F（000） = 1255.0,Mu（mm-1） = 1.756,λ（MoKα） = 0.71073 ,R = 0.0625 and wR = 0.1952.In 1,the [V12B18O54（OH）6]8- units are connected by [Cu（en）2]2＋,binuclear Na（1） and Na（2） to form a three-dimensional porous framework.展开更多
Evaluating the hydrocarbon generation potential of highly mature organic matter is a key and critically challenging area of research in petroleum geochemistry. To explore this issue, we used negative ion electrospray ...Evaluating the hydrocarbon generation potential of highly mature organic matter is a key and critically challenging area of research in petroleum geochemistry. To explore this issue, we used negative ion electrospray ionization-Fourier transform-ion cyclotron resonance-mass spectrometry to investigate the molecular evolution of N-containing compounds in Carboniferous-lower Permian source rocks with a range of maturities in the northwestern Junggar Basin, China. The N1compounds formed from on-fluorescent chlorophyll catabolites(NCCs), which record the characteristics of the residual soluble organic matter. These components remain in the source rocks after hydrocarbon generation and expulsion, and enable evaluation of the hydrocarbon generation potential. The newly defined indexes of molecular evolution, which are the polymerization index P1([DBE 18+DBE 15]/[DBE 12+DBE 9]_N1) and alkylation index R1(RC_(6–35)/RC_(0–5)), combined with the vitrinite reflectance(VR_(o)) and paleo-salinity index(β-carotane/n Cmax), can identify the factors that control the evolution of highly mature organic matter. The main factor for source rocks deposited in a weakly saline environment is the maturity, but for a highly saline environment both the maturity and salinity are key factors. The high salinity inhibits the molecular polymerization of organic matter and extends the oil generation peak. Given the differences in the bio-precursors in saline source rocks, we propose a new model for hydrocarbon generation that can be used to determine the oil generation potential of highly mature organic matter.展开更多
Two N-containing borates, BTES and BMES, were synthesized with dodecyl phenol, 2-(N-containing heterocyclic) ethan-1-ol, boric acid, and dibutylamine, and their tribological properties in rapeseed oil(RSO) were invest...Two N-containing borates, BTES and BMES, were synthesized with dodecyl phenol, 2-(N-containing heterocyclic) ethan-1-ol, boric acid, and dibutylamine, and their tribological properties in rapeseed oil(RSO) were investigated using a four-ball tester. The results showed that the load-carrying ability(P_B value) of RSO can be improved by 40.9% and 67.9%, respectively, when using 0.5 wt% BTES and BMES. Moreover, the antiwear and friction-reducing performances of the additive-containing oils increased with the additive concentration. The X-ray photoelectron spectroscopy results of the worn steel ball surfaces showed that BTES and BMES formed protective films, which contained boron oxide, iron oxide, ferrous sulfate, ferrous sulfide(for BMES), and other organic nitrogen compounds, on the metal surfaces. The better load-carrying and antiwear performances of BMES than those of BTES might be due to their different sulfur contents, which result in different tribochemical reaction films on the contact surfaces. The oxidation stability tests showed that BTES and BMES possessed synergistic antioxidation activity with N-phenyl-α-naphthylamine(T531), and consequently, the oxidation activation energy of the oil sample increased by 77.85% and 82.19%, respectively, compared with that of RSO when the oil sample contained 0.05 wt% BTES/BMES and 0.25% T531.展开更多
基金financial support from the National Natural Science Foundation of China (51764048, 21961030 and 51474191)Yunnan Province Thousand Youth Talents Plan+1 种基金the Application Basis Research Project of Yunnan Province Science and Technology Department (2017FD144)the Key Natural Science Foundation of Yunnan Province China (2018FA28, 2019FY003023 and 2018FH001-007)。
文摘Organic electrode materials are desirable for green and sustainable Li-ion batteries(LIBs) due to their light-weight, low cost, abundance and multi-electron transfer reactions during battery operation. However, the successful utilization of organic electrodes is hindered by their poor electrical conductivity and low cyclic stability. Herein, a facile synthesis of π-conjugated N-containing heteroaromatic hexacarboxylate(Li6-HAT) compound and its electrochemical performance as an anode material in LIBs is reported.The as-synthesized Li6-HAT electrode renders an ultrahigh initial capacity of 1126.3 m Ah g^(-1) at the current density of 100 m A g^(-1). Moreover, π-conjugated N-containing heteroaromatic center provide excellent reversibility of(de)lithiation process, resulting in excellent capacity retention. Furthermore, a combination of density functional theory(DFT) calculations, in-situ Fourier transform infrared(FTIR) and ex-situ X-ray photoelectron spectroscopy(XPS) characterization reveal that the π-conjugated nitrogen and carboxyl oxygen act as electrochemically active sites during the charge/discharge process. The current work provides novel insights into the charge storage mechanism of organic electrodes and opens up avenues for further development and utilization of organic electrodes in Li-ion batteries.
基金supported by the Ningbo Natural Science Foundation (2009A610052)the "Qianjiang Talent" Programs of Zhejiang Province (2009R10032)the K. C. Wang Magna Fund in Ningbo University
文摘A novel inorganic-organic hybrid borate,[Al2（fum）（H3BO3）（OH） 4]n·n（H3BO3） （1,H2fum = fumaric acid） ,has been synthesized and characterized by single-crystal X-ray diffraction,FTIR and elemental analysis. Crystal data for compound 1： orthorhombic,space group Pnma,a = 14.108（3） ,b = 6.9412（14） ,c = 14.995（3）A,V = 1468.3（5）A^3,Z = 4,Mr = 359.72,Dc = 1.627 g/cm^3,μ = 0.254 mm^-1,F（000） = 736,the final R = 0.0492 and wR = 0.1650 with I 〉 2σ（I） . In compound 1,each Al^Ⅲ ion is coordinated by six oxygen atoms to adopt a distorted octahedral geometry. Both fumarate anion and the coordinated boric acid act as bidentate bridging ligands to link two neighboring Al^Ⅲ centers simultaneously. Each Al^Ⅲ ion is bridged by two μ2-hydroxyl ligands to construct an infinite wave-like [Al2（fum）（H3BO3）（OH） 4]n chain. These one-dimensional chains form hydrogen bonds with free boric acid molecules giving rise to a three-dimensional supramolecular network.
基金Funded by Chinese Natural Science Foundation Committee(No.50673080)
文摘A series of thermoreversible konjac glucomannan gels crosslinked by organic borate were prepared. Required amount of hydrophilic SiO2 was added into the konjac glucomannan solutions before the crosslinking reaction, The gel network was formed through the crosslinking reaction between borate ions dissociated from organic borate and the cis-diol hydroxyl groups on the mannose units of polysaccharide chains. The rheological properties of the complex gels were studied by dynamic viscoelastic measurement. The gelation kinetics of the complex gels was studied and the critical getation points of the gels were exactly determined by the Winter-Chambon criterion. The effects of temperature and composite ratio on the shear storage modulus （G＇）, the loss modulus （G＂） and the sol-gel transition points were investigated.
基金supported by the National Natural Science Foundation of China (20873021,21003020)Doctoral Fund of Ministry of Education of China (20093514120002)New Century Excellent Talent Supported Plan of Fujian Province (SXSJRC2007-21)
文摘A polyoxovanadium borate [Na（H2O）]2[Na（H2O）2]2[Cu（en）2][V12B18O54（OH）6]·（H3O）2·（H2O）18 1（en = ethylenediamine） has been hydrothermally synthesized and characterized by IR,two-dimensional infrared（2D IR） correlation spectroscopy with magnetic and thermal perturba-tion,thermal IR spectroscopy,thermal gravimetric analysis and single-crystal X-ray diffraction.It crystallizes in triclinic,space group P with a = 12.981（3）,b = 13.044（3）,c = 14.208（3） ,α = 63.98（3）,β = 77.17（3）,γ = 14.208（3）°,V = 2001.0（8） 3,Z = 1,Mr = 2518.05,Dc = 2.090 g/cm-1,F（000） = 1255.0,Mu（mm-1） = 1.756,λ（MoKα） = 0.71073 ,R = 0.0625 and wR = 0.1952.In 1,the [V12B18O54（OH）6]8- units are connected by [Cu（en）2]2＋,binuclear Na（1） and Na（2） to form a three-dimensional porous framework.
基金supported by the National Natural Science Foundation of China(Grant Nos.42230808 and 42102148)China Postdoctoral Science Foundation(Grant No.2021M691497)。
文摘Evaluating the hydrocarbon generation potential of highly mature organic matter is a key and critically challenging area of research in petroleum geochemistry. To explore this issue, we used negative ion electrospray ionization-Fourier transform-ion cyclotron resonance-mass spectrometry to investigate the molecular evolution of N-containing compounds in Carboniferous-lower Permian source rocks with a range of maturities in the northwestern Junggar Basin, China. The N1compounds formed from on-fluorescent chlorophyll catabolites(NCCs), which record the characteristics of the residual soluble organic matter. These components remain in the source rocks after hydrocarbon generation and expulsion, and enable evaluation of the hydrocarbon generation potential. The newly defined indexes of molecular evolution, which are the polymerization index P1([DBE 18+DBE 15]/[DBE 12+DBE 9]_N1) and alkylation index R1(RC_(6–35)/RC_(0–5)), combined with the vitrinite reflectance(VR_(o)) and paleo-salinity index(β-carotane/n Cmax), can identify the factors that control the evolution of highly mature organic matter. The main factor for source rocks deposited in a weakly saline environment is the maturity, but for a highly saline environment both the maturity and salinity are key factors. The high salinity inhibits the molecular polymerization of organic matter and extends the oil generation peak. Given the differences in the bio-precursors in saline source rocks, we propose a new model for hydrocarbon generation that can be used to determine the oil generation potential of highly mature organic matter.
基金the financial support provided by the National Natural Science Foundation of China(Nos.21563012 and 21363008)Jiangsu Provincial Natural Science Foundation of China(No.BK20161188)+1 种基金Jiangxi Natural Science Foundation of China(Nos.20143ACB20003,20162BCB22020 and 20171BCD40009)Jiangxi Provincial Education Department Foundation of China(No.GJJ170371)
文摘Two N-containing borates, BTES and BMES, were synthesized with dodecyl phenol, 2-(N-containing heterocyclic) ethan-1-ol, boric acid, and dibutylamine, and their tribological properties in rapeseed oil(RSO) were investigated using a four-ball tester. The results showed that the load-carrying ability(P_B value) of RSO can be improved by 40.9% and 67.9%, respectively, when using 0.5 wt% BTES and BMES. Moreover, the antiwear and friction-reducing performances of the additive-containing oils increased with the additive concentration. The X-ray photoelectron spectroscopy results of the worn steel ball surfaces showed that BTES and BMES formed protective films, which contained boron oxide, iron oxide, ferrous sulfate, ferrous sulfide(for BMES), and other organic nitrogen compounds, on the metal surfaces. The better load-carrying and antiwear performances of BMES than those of BTES might be due to their different sulfur contents, which result in different tribochemical reaction films on the contact surfaces. The oxidation stability tests showed that BTES and BMES possessed synergistic antioxidation activity with N-phenyl-α-naphthylamine(T531), and consequently, the oxidation activation energy of the oil sample increased by 77.85% and 82.19%, respectively, compared with that of RSO when the oil sample contained 0.05 wt% BTES/BMES and 0.25% T531.
