Marine biofouling is an urgent global problem in the process of ocean exploitation and utilization.In our work,a series of zinc-based acrylate copolymers(ACZn-x)were designed and synthesized using benzoic acid,zinc ox...Marine biofouling is an urgent global problem in the process of ocean exploitation and utilization.In our work,a series of zinc-based acrylate copolymers(ACZn-x)were designed and synthesized using benzoic acid,zinc oxide(ZnO)and a random quaternion copolymer consisting of ethyl acrylate(EA),butyl acrylate(BA),acrylic acid(AA)and methacrylic acid(MAA)by free radical polymerization and dehydration condensation.The ACZn-x with a zinc benzoate side chain is able to hydrolyze in natural seawater under static conditions,resulting in the formation of a smooth surface.We investigated and confirmed the antifouling(AF)behavior of ACZn-x in the laboratory and revealed that they have better antibacterial(86%for S.aureus and 72%for E.coli)and anti-algal(≥60.1%for N.closterium and≥67.5%for P.subcordiformis)activities.We also assessed the marine AF properties of ACZn-x and corresponding coatings in Qingdao,China;the ACZn-x exhibited ideal AF properties with little silt and biological mucosa adhered to the ACZn-x surface after 6 months,and corresponding coatings exhibited little biofouling after 16 months in the ocean.Importantly,possible AF mechanisms were further proposed at the cellular level.These results could be helpful for the development and application of effective AF coatings.展开更多
Carboxymethyl starch/silver oxide nanocomposites(CMS-Ag_(2)O NCs)were successfully fabricated by modifying carboxymethyl starch(CMS)with Ag_(2)O obtained from an aqueous AgNO_(3)solution as silver source.Ag_(2)O nanop...Carboxymethyl starch/silver oxide nanocomposites(CMS-Ag_(2)O NCs)were successfully fabricated by modifying carboxymethyl starch(CMS)with Ag_(2)O obtained from an aqueous AgNO_(3)solution as silver source.Ag_(2)O nanoparticles(NPs)formed on the surface of CMS by ion exchange.Based on SEM images,the diameters of Ag_(2)O NPs were determined to be between 50 and 100 nm.From the XRD spectra of CMS-Ag_(2)O NCs,the new diffraction peaks appeared at 33.88°and 38.08°,which were attributed to the Ag_(2)O NPs.According to the XPS analysis,Ag 3d_(5/2)and Ag 3d_(3/2)peaks in CMS-Ag_(2)O NCs were fitted into two main peaks centered at 367.6 eV and 373.6 eV,which were attributed to Ag^(+).The antibacterial efficiencies of CMS-Ag_(2)O NCs against Escherichia coli,Staphylococcus aureus,Pseudoalteromonas tetraodonis,Micrococcus luteus,and Shewanella putrefaciens were determined to be 99.6%,99.7%,99.4%,99.5%,and 99.6%,respectively.The antibacterial efficiencies of CMS-Ag_(2)O NCs against the bacterial species were all greater than 99%.Therefore,these results indicated that CMS-Ag_(2)O NCs was highly effective as a bactericidal agent against multiple bacterial species.CMS-Ag_(2)O NCs can be further applied to antifouling coating.展开更多
以实验室自主合成的辣素类化合物——N-(4-羟基-2-甲基-5-甲硫基苄基)丙烯酰胺(HMMBA)为功能单体,通过与丙烯酸酯类单体的自由基聚合反应,合成出侧链悬挂辣素衍生结构的丙烯酸树脂,采用红外光谱(IR)和核磁氢谱(1 H NMR)对其结构进行了...以实验室自主合成的辣素类化合物——N-(4-羟基-2-甲基-5-甲硫基苄基)丙烯酰胺(HMMBA)为功能单体,通过与丙烯酸酯类单体的自由基聚合反应,合成出侧链悬挂辣素衍生结构的丙烯酸树脂,采用红外光谱(IR)和核磁氢谱(1 H NMR)对其结构进行了表征。考察了引发剂用量、聚合温度、聚合时间对树脂合成的影响,并确定了树脂的最佳合成条件为,引发剂用量为单体质量的1.5%,聚合温度为100℃,聚合时间为8h。以自然界常见细菌大肠杆菌作为受试菌对所合成的树脂进行了抗菌性能测试,实验结果表明,随着HMMBA含量的增加,树脂的抗菌率也相应增大。展开更多
以取代芳烃和N-羟甲基丙烯酰胺为原料,采用傅克烷基化反应合成了四种含辣素衍生结构单体:4-羟基-2-甲基-5-甲硫基苄基丙烯酰胺(A)、2-羟基-4-丙烯酰胺甲基-5-甲硫基-6-甲基苄基丙烯酰胺(B)、3-丙烯酰胺甲基-2-羟基苯甲酰胺(C)和1-丙烯...以取代芳烃和N-羟甲基丙烯酰胺为原料,采用傅克烷基化反应合成了四种含辣素衍生结构单体:4-羟基-2-甲基-5-甲硫基苄基丙烯酰胺(A)、2-羟基-4-丙烯酰胺甲基-5-甲硫基-6-甲基苄基丙烯酰胺(B)、3-丙烯酰胺甲基-2-羟基苯甲酰胺(C)和1-丙烯酰胺甲基-2-萘酚(D),并通过红外光谱(IR)和核磁氢谱(1 H NMR)对其结构进行了表征。抑菌实验结果表明化合物D对两种受试菌(金黄色葡萄球菌和大肠杆菌)的抑制活性最高,最小抑菌浓度均可达到0.187 5mg/mL,且D对两种受试藻(三角褐指藻和新月菱形藻)的抑制活性也最高。以四种化合物为功能单体合成出树脂,树脂对受试藻均具有较高的抑制活性,含化合物D的树脂的抑制活性最高,72h后抑制率均可达到50%以上。展开更多
Enzyme-based antifouling coatings are potential alternative to traditional tributyltin-based coatings in the marine biofouling control depended on its environmental friendliness.Proteases are usually the key antifouli...Enzyme-based antifouling coatings are potential alternative to traditional tributyltin-based coatings in the marine biofouling control depended on its environmental friendliness.Proteases are usually the key antifouling active components in enzyme based antifouling coatings.In this work,based on biological antagonism effect,a marine proteolytic bacterial strain of Bacillus velezensis was isolated from the sea mud,and denoted as SM-1.The scanning electron microscope(SEM)revealed that the bacteria are rod-shaped with length 1-1.3μm.The protease-producing conditions of SM-1 were investigated,and it was found that the culture solution displays higher proteolytic activity under the culture conditions of 35℃,10‰-20‰salinity,pH 6-9 and more than 7 d culture time.Moreover,the 25 kDa protein was confirmed to be the main active component in the crude protease,which was revealed via the experiment of SDS-PAGE.The antifouling assay indicated that the protease SM-1 has remarkable effect on the decomposition of barnacle cement and diatom secretion,and also can effectively inhibit the attachment of barnacle cyprids,diatom and mussel byssus.Therefore,this protease potentially can be used as environmental-friendly antifoulant of enzyme-based marine antifouling coatings,and this work also provides a new approach to obtain antifouling protease via isolating proteolytic bacteria from the sea mud surrounding representative fouling organisms.展开更多
PANI copolymer micro/nanostructures with different surface wettability were obtained from the chemical oxidation copolymerization of aniline(Ani)with 2-ethyl aniline(EA)at diverse[EA]/[Ani+EA]molar ratios,by employing...PANI copolymer micro/nanostructures with different surface wettability were obtained from the chemical oxidation copolymerization of aniline(Ani)with 2-ethyl aniline(EA)at diverse[EA]/[Ani+EA]molar ratios,by employing ammonium persulfate as an oxidant.The results revealed that the poly(aniline-co-2-ethyl aniline)(PANI-EA)copolymer micro/nanostructures exhibited satisfactory anticorrosion performance for carbon steel,and the corrosion protection efficiency increased with the increase of water repellent property.Poly(2-ethyl aniline)(PEA)showed the largest contact angle(CA=145°)and show the best corrosion protection for the carbon steel(h=87.29%).It is found that the superior anticorrosion property of PEA is attributed to its high hydrophobicity,low conductivity and low porosity.展开更多
The pursuit of high oil recovery rate has been a persistent objective for oil industry. Pseudomonas sp. LP-7 and Bacillus sp. PAH-2 were isolated from oil-contaminated surface soil samples of an oilfield. The antimicr...The pursuit of high oil recovery rate has been a persistent objective for oil industry. Pseudomonas sp. LP-7 and Bacillus sp. PAH-2 were isolated from oil-contaminated surface soil samples of an oilfield. The antimicrobial degradation rates(ADRs) of polymers achieved by LP-7 and PAH-2 were evaluated at a temperature of 35 °C in the mineral salt media during the shaken flask trial. The ADRs of copolymer synthesized by using a surfactant with a concentration of 5% could reach 8.4% for PAH-2 and 15.3% for LP-7. The ADRs of copolymer could reach 10.4% for PAH-2 and 21.3% for LP-7,when the polymer concentration was 2 g/L. All results confirmed that the ADRs of copolymers increased with an increasing content of HDDE(capsaicin derivative monomer) in the polymer. The copolymers also manifested excellent antimicrobial degradation performance in the presence of Cu^(2+), Zn^(2+), and Pb^(2+) ions, respectively, which had great potential for applications in enhanced oil recovery.展开更多
As a group of diversified frameworks, quinazolin derivatives displayed a broad field of biological functions, especially as anticancer. To investigate the quantitative structure-activity relationship, 3D-QSAR models ...As a group of diversified frameworks, quinazolin derivatives displayed a broad field of biological functions, especially as anticancer. To investigate the quantitative structure-activity relationship, 3D-QSAR models were generated with 24 quinazolin scaffold molecules. The experimental and predicted pIC50 values for both training and test set compounds showed good correlation, which proved the robustness and reliability of the generated QSAR models. The most effective CoMFA and CoMSIA were obtained with correlation coefficient2ncv r of 1.00 (both) and leave-one-out coefficient q2 of 0.61 and 0.59, respectively. The predictive abilities of CoMFA and CoMSIA were quite good with the predictive correlation coefficients (2pred r ) of 0.97 and 0.91. In addition, the statis-tic results of CoMFA and CoMSIA were used to design new quinazolin molecules.展开更多
Abstract Goethite widely exists among ocean sediments; it plays an important role in fixing heavy metals and adsorbing organic contaminants. So the understanding of the adsorbing process of water molecule on its surfa...Abstract Goethite widely exists among ocean sediments; it plays an important role in fixing heavy metals and adsorbing organic contaminants. So the understanding of the adsorbing process of water molecule on its surface will be very helpful to further reveal such environmental friendly processes. The configuration, electronic properties and interaction energy of water molecules adsorbed on pnma goethite (010) surface were investigated in detail by using density functional theory on 6-31G (d,p) basis set and projec- tor-augment wave (PAW) method. The mechanism of the interaction between goethite surface and H20 was proposed. Despite the differences in total energy, there are four possible types of water molecule adsorption configurations on goethite (010) surface (Aa, Ab, Ba, Bb), forming coordination bond with surface Fe atom. Results of theoretical modeling indicate that the dissociation process of adsorbed water is an endothermic reaction with high activation energy. The dissociation of adsorbed water molecule is a proton transportation process between water's O atoms and surface. PDOS results indicate that the bonding between 1-120 and (010) surface is due to the overlapping of water's 2p orbitals and Fe's 3d orbitals. These results clarify the mechanism on how adsorbed water is dissociated on the surface of goethite and potentially provide useful information of the surface chemistry of goethite.展开更多
基金supported by the National Key Research and Development Project(No.2019YFC0312101)the Scientific Research Project of Sanya Yazhou Bay Science and Technology City Administration(No.SKJC2020-01-015)the Hainan Provincial Key Research and Development Project(No.ZDYF2021GXJS029)。
文摘Marine biofouling is an urgent global problem in the process of ocean exploitation and utilization.In our work,a series of zinc-based acrylate copolymers(ACZn-x)were designed and synthesized using benzoic acid,zinc oxide(ZnO)and a random quaternion copolymer consisting of ethyl acrylate(EA),butyl acrylate(BA),acrylic acid(AA)and methacrylic acid(MAA)by free radical polymerization and dehydration condensation.The ACZn-x with a zinc benzoate side chain is able to hydrolyze in natural seawater under static conditions,resulting in the formation of a smooth surface.We investigated and confirmed the antifouling(AF)behavior of ACZn-x in the laboratory and revealed that they have better antibacterial(86%for S.aureus and 72%for E.coli)and anti-algal(≥60.1%for N.closterium and≥67.5%for P.subcordiformis)activities.We also assessed the marine AF properties of ACZn-x and corresponding coatings in Qingdao,China;the ACZn-x exhibited ideal AF properties with little silt and biological mucosa adhered to the ACZn-x surface after 6 months,and corresponding coatings exhibited little biofouling after 16 months in the ocean.Importantly,possible AF mechanisms were further proposed at the cellular level.These results could be helpful for the development and application of effective AF coatings.
基金supported by the National Key Research and Development Project(No.2019YFC0312103)the Open Fund of Shandong Key Laboratory of Corrosion Science(No.KLCS201905)。
文摘Carboxymethyl starch/silver oxide nanocomposites(CMS-Ag_(2)O NCs)were successfully fabricated by modifying carboxymethyl starch(CMS)with Ag_(2)O obtained from an aqueous AgNO_(3)solution as silver source.Ag_(2)O nanoparticles(NPs)formed on the surface of CMS by ion exchange.Based on SEM images,the diameters of Ag_(2)O NPs were determined to be between 50 and 100 nm.From the XRD spectra of CMS-Ag_(2)O NCs,the new diffraction peaks appeared at 33.88°and 38.08°,which were attributed to the Ag_(2)O NPs.According to the XPS analysis,Ag 3d_(5/2)and Ag 3d_(3/2)peaks in CMS-Ag_(2)O NCs were fitted into two main peaks centered at 367.6 eV and 373.6 eV,which were attributed to Ag^(+).The antibacterial efficiencies of CMS-Ag_(2)O NCs against Escherichia coli,Staphylococcus aureus,Pseudoalteromonas tetraodonis,Micrococcus luteus,and Shewanella putrefaciens were determined to be 99.6%,99.7%,99.4%,99.5%,and 99.6%,respectively.The antibacterial efficiencies of CMS-Ag_(2)O NCs against the bacterial species were all greater than 99%.Therefore,these results indicated that CMS-Ag_(2)O NCs was highly effective as a bactericidal agent against multiple bacterial species.CMS-Ag_(2)O NCs can be further applied to antifouling coating.
文摘以实验室自主合成的辣素类化合物——N-(4-羟基-2-甲基-5-甲硫基苄基)丙烯酰胺(HMMBA)为功能单体,通过与丙烯酸酯类单体的自由基聚合反应,合成出侧链悬挂辣素衍生结构的丙烯酸树脂,采用红外光谱(IR)和核磁氢谱(1 H NMR)对其结构进行了表征。考察了引发剂用量、聚合温度、聚合时间对树脂合成的影响,并确定了树脂的最佳合成条件为,引发剂用量为单体质量的1.5%,聚合温度为100℃,聚合时间为8h。以自然界常见细菌大肠杆菌作为受试菌对所合成的树脂进行了抗菌性能测试,实验结果表明,随着HMMBA含量的增加,树脂的抗菌率也相应增大。
文摘以取代芳烃和N-羟甲基丙烯酰胺为原料,采用傅克烷基化反应合成了四种含辣素衍生结构单体:4-羟基-2-甲基-5-甲硫基苄基丙烯酰胺(A)、2-羟基-4-丙烯酰胺甲基-5-甲硫基-6-甲基苄基丙烯酰胺(B)、3-丙烯酰胺甲基-2-羟基苯甲酰胺(C)和1-丙烯酰胺甲基-2-萘酚(D),并通过红外光谱(IR)和核磁氢谱(1 H NMR)对其结构进行了表征。抑菌实验结果表明化合物D对两种受试菌(金黄色葡萄球菌和大肠杆菌)的抑制活性最高,最小抑菌浓度均可达到0.187 5mg/mL,且D对两种受试藻(三角褐指藻和新月菱形藻)的抑制活性也最高。以四种化合物为功能单体合成出树脂,树脂对受试藻均具有较高的抑制活性,含化合物D的树脂的抑制活性最高,72h后抑制率均可达到50%以上。
基金supported by the National Basic Research Program of China (No. 2014CB643305)the National Natural Science Foundation of China (No. 213 01161)
文摘Enzyme-based antifouling coatings are potential alternative to traditional tributyltin-based coatings in the marine biofouling control depended on its environmental friendliness.Proteases are usually the key antifouling active components in enzyme based antifouling coatings.In this work,based on biological antagonism effect,a marine proteolytic bacterial strain of Bacillus velezensis was isolated from the sea mud,and denoted as SM-1.The scanning electron microscope(SEM)revealed that the bacteria are rod-shaped with length 1-1.3μm.The protease-producing conditions of SM-1 were investigated,and it was found that the culture solution displays higher proteolytic activity under the culture conditions of 35℃,10‰-20‰salinity,pH 6-9 and more than 7 d culture time.Moreover,the 25 kDa protein was confirmed to be the main active component in the crude protease,which was revealed via the experiment of SDS-PAGE.The antifouling assay indicated that the protease SM-1 has remarkable effect on the decomposition of barnacle cement and diatom secretion,and also can effectively inhibit the attachment of barnacle cyprids,diatom and mussel byssus.Therefore,this protease potentially can be used as environmental-friendly antifoulant of enzyme-based marine antifouling coatings,and this work also provides a new approach to obtain antifouling protease via isolating proteolytic bacteria from the sea mud surrounding representative fouling organisms.
基金financial supports of the National Natural Science Foundation of China (No. 41476059)the Natural Science Foundation of Hebei Province (No. E2018108011)
文摘PANI copolymer micro/nanostructures with different surface wettability were obtained from the chemical oxidation copolymerization of aniline(Ani)with 2-ethyl aniline(EA)at diverse[EA]/[Ani+EA]molar ratios,by employing ammonium persulfate as an oxidant.The results revealed that the poly(aniline-co-2-ethyl aniline)(PANI-EA)copolymer micro/nanostructures exhibited satisfactory anticorrosion performance for carbon steel,and the corrosion protection efficiency increased with the increase of water repellent property.Poly(2-ethyl aniline)(PEA)showed the largest contact angle(CA=145°)and show the best corrosion protection for the carbon steel(h=87.29%).It is found that the superior anticorrosion property of PEA is attributed to its high hydrophobicity,low conductivity and low porosity.
基金the Natural Science Foundation of China(50673085,41576077)the National High-Tech Research and Development Programme of China(2010AA09Z203)the Fundamental Research Funds for the Central Universities of China(201562026)
文摘The pursuit of high oil recovery rate has been a persistent objective for oil industry. Pseudomonas sp. LP-7 and Bacillus sp. PAH-2 were isolated from oil-contaminated surface soil samples of an oilfield. The antimicrobial degradation rates(ADRs) of polymers achieved by LP-7 and PAH-2 were evaluated at a temperature of 35 °C in the mineral salt media during the shaken flask trial. The ADRs of copolymer synthesized by using a surfactant with a concentration of 5% could reach 8.4% for PAH-2 and 15.3% for LP-7. The ADRs of copolymer could reach 10.4% for PAH-2 and 21.3% for LP-7,when the polymer concentration was 2 g/L. All results confirmed that the ADRs of copolymers increased with an increasing content of HDDE(capsaicin derivative monomer) in the polymer. The copolymers also manifested excellent antimicrobial degradation performance in the presence of Cu^(2+), Zn^(2+), and Pb^(2+) ions, respectively, which had great potential for applications in enhanced oil recovery.
基金financial supports from the National Natural Science Foundation of China (Nos. 50673085, 20677053)the National High-Tech Research and Development Programme of China (No. 2010AA09Z203)
文摘As a group of diversified frameworks, quinazolin derivatives displayed a broad field of biological functions, especially as anticancer. To investigate the quantitative structure-activity relationship, 3D-QSAR models were generated with 24 quinazolin scaffold molecules. The experimental and predicted pIC50 values for both training and test set compounds showed good correlation, which proved the robustness and reliability of the generated QSAR models. The most effective CoMFA and CoMSIA were obtained with correlation coefficient2ncv r of 1.00 (both) and leave-one-out coefficient q2 of 0.61 and 0.59, respectively. The predictive abilities of CoMFA and CoMSIA were quite good with the predictive correlation coefficients (2pred r ) of 0.97 and 0.91. In addition, the statis-tic results of CoMFA and CoMSIA were used to design new quinazolin molecules.
基金financial supports from the National Natural Science Foundation of China (Nos.50673085,20677053)
文摘Abstract Goethite widely exists among ocean sediments; it plays an important role in fixing heavy metals and adsorbing organic contaminants. So the understanding of the adsorbing process of water molecule on its surface will be very helpful to further reveal such environmental friendly processes. The configuration, electronic properties and interaction energy of water molecules adsorbed on pnma goethite (010) surface were investigated in detail by using density functional theory on 6-31G (d,p) basis set and projec- tor-augment wave (PAW) method. The mechanism of the interaction between goethite surface and H20 was proposed. Despite the differences in total energy, there are four possible types of water molecule adsorption configurations on goethite (010) surface (Aa, Ab, Ba, Bb), forming coordination bond with surface Fe atom. Results of theoretical modeling indicate that the dissociation process of adsorbed water is an endothermic reaction with high activation energy. The dissociation of adsorbed water molecule is a proton transportation process between water's O atoms and surface. PDOS results indicate that the bonding between 1-120 and (010) surface is due to the overlapping of water's 2p orbitals and Fe's 3d orbitals. These results clarify the mechanism on how adsorbed water is dissociated on the surface of goethite and potentially provide useful information of the surface chemistry of goethite.