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NiCo/Al_(2)O_(3)nanocatalysts for the synthesis of 5-amino-1-pentanol and 1,5-pentanediol from biomass-derived 2-hydroxytetrahydropyran

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Green Chemical Engineering 2024年第1期5卷 119-131页

作者： jian Yang jia Zhang Enrico Benassi Xuemei Li hailong Liu Weiguo Fang Junying Tian Chungu Xia Zhiwei Huang State Key Laboratory for Oxo Synthesis and Selective Oxidation Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou730000China School of Petrochemical Engineering Lanzhou University of TechnologyLanzhou730050China Novosibirsk State University Novosibirsk630090Russia University of Chinese Academy of Sciences Beijing100049China

Al_(2)O_(3)-supported monometallic Ni,Co,and bimetallic Ni-Co nanocatalysts originated from layered double hydroxide precursors were synthesized by co-precipitation method,and used for the synthesis of useful 5-amino-1-pentanol(5-AP)and 1,5-pentanediol(1,5-PD)by reductive amination(RA)or direct hydrogenation of biofurfuralderived 2-hydroxytetrahydropyran(2-HTHP),respectively.In both reactions,the yield of the target products decreased monotonously with the increasing amounts of Co in the NiCo/Al_(2)O_(3)catalysts,owing probably to the replacement of highly reactive Ni by Co component with inferior hydrogenation activity at the low reaction temperature of 60℃.However,the incorporation of Co could improve the reducibility of the NiCo/Al_(2)O_(3)bimetallic catalysts and promote the reaction stability of the catalysts,especially for Ni_(2)Co1/Al_(2)O_(3),in both reactions with over 180 h time-on-stream.Characterization of the catalysts before and after the reaction showed that the incorporating Co could inhibit the sintering of metal particles and hinder the surface oxidation of the more reactive Ni0species,thanks to the formation of Ni-Co alloy in the bimetallic catalysts.DFT-based modeling of the reaction mechanisms is also performed,supporting the reaction pathway proposed previously and also the much higher activity of Ni in the RA of 2-HTHP as compared with Co.

关键词： NiCo bimetallic catalysts Layered double hydroxide Reductive amination Amino alcohol Quantum chemical calculations

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Natural attapulgite supported nano-Ni catalysts for the efficient reductive amination of biomass-derived aldehydes and ketones

Green Synthesis and Catalysis

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Green Synthesis and Catalysis 2024年第1期5卷 42-50页

作者： jia Zhang jian Yang Xuemei Li Bin Mu hailong Liu Chungu Xia Aiqin Wang Zhiwei Huang State Key Laboratory for Oxo Synthesis and Selective Oxidation Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou 730000China Key Laboratory of Clay Mineral Applied Research of Gansu Province Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou 730000China University of Chinese Academy of Sciences Beijing 100049China

The efficient synthesis of useful primary amines via reductive amination of biomass-based aldehydes and ketones over earth-abundant base metal catalysts is an attractive biomass value-adding technology yet facing lots of challenges.Herein,natural attapulgite(ATP)was applied as support for the fabrication of active Ni catalysts with different Ni loadings(5–30 wt%)by the deposition-precipitation method.The Ni/ATP-550 catalyst with 10–15 wt%Ni loadings was found to present the highest catalytic performance for the synthesis of valuable 5-amino-1-pentanol(5-AP)via reductive amination of biofurfural-derived 2-hydroxytetrahydropyran among a variety of commonly used oxide supports loaded Ni catalysts,as well as ATP supported nickel catalysts with other loadings,achieving 5-AP yield up to 94%.The intrinsic activity of the Ni/ATP catalysts was found to depend strongly on the Ni^(0) crystallite size and Ni^(0) fraction of the catalysts,which generally increased with increasing Ni^(0) crystallite size and fraction,owing probably to the hydrogenation of imine intermediate is a structure-sensitive reaction.The efficient 10Ni/ATP-550 catalyst also exhibited good activity and stability in the reductive amination of several other biomass-derived aldehydes and ketones to their corresponding primary amines with good to excellent yields(81%–99%).This work provided a clean and efficient natural ATP-supported non-noble metal nickel-based catalytic system for the reductive amination of aldehydes and ketones to synthesize high-value-added primary amines,which could be a promising candidate for the industrial production of amines.

关键词： Attapulgite Nano-Ni catalyst Reductive amination 5-Amino-1-pentanol Structure-activity relationship

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Prediction of Porous Media Fluid Flow with Spatial Heterogeneity Using Criss-Cross Physics-Informed Convolutional Neural Networks

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Computer Modeling in Engineering & Sciences 2024年第2期138卷 1323-1340页

作者： jiangxia Han Liang Xue Ying jia Mpoki Sam Mwasamwasa Felix Nanguka Charles Sangweni hailong Liu Qian Li State Key Laboratory of Petroleum Resources and Prospecting China University of PetroleumBeijing102249China Department of Oil-Gas Field Development Engineering College of Petroleum EngineeringChina University of PetroleumBeijing102249China Exploration Production Research Institute SinopecBeijing102249China Ministry of Energy Tanzania Petroleum Development CorporationTowerDar es Salaam2774Tanzania Ministry of Energy Building Petroleum Upstream Regulatory Authority in Tanzania(PURA)Dar es Salaam11439Tanzania

Recent advances in deep neural networks have shed new light on physics,engineering,and scientific computing.Reconciling the data-centered viewpoint with physical simulation is one of the research hotspots.The physicsinformedneural network(PINN)is currently the most general framework,which is more popular due to theconvenience of constructing NNs and excellent generalization ability.The automatic differentiation(AD)-basedPINN model is suitable for the homogeneous scientific problem;however,it is unclear how AD can enforce fluxcontinuity across boundaries between cells of different properties where spatial heterogeneity is represented bygrid cells with different physical properties.In this work,we propose a criss-cross physics-informed convolutionalneural network(CC-PINN)learning architecture,aiming to learn the solution of parametric PDEs with spatialheterogeneity of physical properties.To achieve the seamless enforcement of flux continuity and integration ofphysicalmeaning into CNN,a predefined 2D convolutional layer is proposed to accurately express transmissibilitybetween adjacent cells.The efficacy of the proposedmethodwas evaluated through predictions of several petroleumreservoir problems with spatial heterogeneity and compared against state-of-the-art(PINN)through numericalanalysis as a benchmark,which demonstrated the superiority of the proposed method over the PINN.

关键词： Physical-informed neural networks(PINN) flow in porous media convolutional neural networks spatial heterogeneity machine learning

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A rolled Mg-8Al-0.5Zn-0.8Ce alloy with high strength-ductility synergy via engineering high-density low angle boundaries

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Journal of Magnesium and Alloys 2022年第10期10卷 2889-2900页

作者： Xiao Ma Min Zha Siqing Wang Yi Yang hailong jia Dan Gao Cheng Wang Huiyuan Wang Key Laboratory of Automobile Materials of Ministry of Education&School of Materials Science and Engineering Nanling CampusJilin UniversityNo.5988 Renmin StreetChangchun 130025PR China State Key Laboratory of Super hard Materials Jilin UniversityChangchun130012PR China International Center of Future Science Jilin UniversityChangchun 130012PR China

Developing low-cost rolled Mg alloys with both high strength and ductility is desirable,while the improved strength is generally accompanied with decreased ductility.Here,by using rotated hard-plate rolling(RHPR)with a total thickness reduction of~85%,we obtained a Mg-8Al-0.5Zn-0.8Ce(wt.%,AZ80-0.8Ce)alloy with a high strength-ductility synergy,i.e.,the yield strength(YS),ultimate tensile strength(UTS)and elongation-to-failure(EF)are~308 MPa,~360 MPa and~13.8%,respectively.It reveals that the high YS is mainly originated from grain boundary strengthening(~212 MPa),followed by dislocation strengthening(~43 MPa)and precipitation hardening(~25 MPa).It is found that a relatively homogeneous fine grain structure containing a large fraction(~62%)of low angle boundaries(LABs)is achieved in the RHPRed alloy,which is benefit for the high tensile EF value.It demonstrates that LABs have important contributions to strengthening and homogenizing tensile deformation process,leading to the simultaneous high strength and high EF.Our work provides a new insight for fabrication of low-cost high performance Mg alloys with an excellent strength-ductility synergy.

关键词： Mg-Al-Zn alloys Rolling Strengthening mechanism Microstructure Strength-ductility synergy

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Photoreduction adjusted surface oxygen vacancy of Bi_(2)MoO_(6) for boosting photocatalytic redox performance

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Frontiers of Chemical Science and Engineering 2023年第12期17卷 1937-1948页

作者： Tie Shi hailong jia Yanmei Feng Bo Gong Daimei Chen Yu Liang Hao Ding Kai Chen Derek Hao Beijing Key Laboratory of Materials Utilization of Nonmetallic Minerals and Solid Wastes National Laboratory of Mineral MaterialsSchool of Materials Science and TechnologyChina University of GeosciencesBeijing 100083China School of Materials Science and Technology Shenyang University of Chemical TechnologyShenyang 110142China Collaborative Innovation Center of Atmospheric Environment and Equipment Technology Jiangsu Key Laboratory of Atmospheric Environment Monitoringand Pollution Control School of Environmental Science and EngineeringNanjing University of Information Science and TechnologyNanjing 210044China Centre for Technology in Water and Wastewater(CTWW) School of Civil and Environmental EngineeringUniversity of Technology Sydney(UTS)NSW 2007Australia

In this study, Bi_(2)MoO_(6) with adjustable rich oxygen vacancies was prepared by a novel and simple solvothermal-photoreduction method which might be suitable for a large-scale production. The experiment results show that Bi_(2)MoO_(6) with rich oxygen vacancies is an excellent photocatalyst. The photocatalytic ability of BMO-10 is 0.3 and 3.5 times higher than that of the pristine Bi_(2)MoO_(6) for Rhodamine B degradation and Cr(VI) reduction, respectively. The results display that the band energy of the samples with oxygen vacancies was narrowed and the light absorption was broadened. Meanwhile, the efficiency of photogenerated electron-holes was increased and the separation and transfer speed of photogenerated carriers were improved. Therefore, this work provides a convenient and efficient method to prepare potential adjustable oxygen vacancy based photocatalysts to eliminate the pollution of dyes and Cr(VI) in water.

关键词： Bi_(2)MoO_(6) oxygen vacancies photoreduction Cr(VI) RhB

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Dislocation behavior in a polycrystalline Mg-Y alloy using multi-scale characterization and VPSC simulation

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Journal of Materials Science & Technology 2022年第3期98卷 87-98页

作者： Bijin Zhou Leyun Wang Jinhui Wang Alireza Maldar Gaoming Zhu hailong jia Peipeng Jin Xiaoqin Zeng Yanjun Li National Engineering Research Center of Light Alloy Net Forming Shanghai Jiao Tong UniversityShanghai 200240China School of Mechanical Engineering Suzhou University of Science and TechnologySuzhou 215009China Department of Materials Science and Engineering Norwegian University of Science and TechnologyTrondheim 7491Norway School of Mechanical Engineering Qinghai UniversityXining 810016China Key Laboratory of Automobile Materials of Ministry of Education&School of Materials Science and Engineering Nanling CampusJilin UniversityChangchun 130025China State Key Laboratory of Metal Matrix Composites Shanghai Jiao Tong UniversityShanghai 200240China

In this study,the dislocation behavior of a polycrystalline Mg-5Y alloy during tensile deformation was quantitatively studied by an in-situ tensile test,visco-plastic self-consistent(VPSC)modeling,and transmission electron microscopy(TEM).The results of the in-situ tensile test show thatdislocations contribute to most of the deformation,while a small fraction ofdislocations are also activated near grain boundaries(GBs).The critical resolved shear stresses(CRSSs)of different dislocation slip systems were estimated.The CRSS ratio between prismatic and basaldislocation slip in the Mg-Y alloy(~13)is lower than that of pure Mg(~80),which is considered as a major reason for the high ductility of the alloy.TEM study shows that thedislocations in the alloy have high mobility,which also helps to accommodate the deformation near GBs.

关键词： Mg-Y alloy Dislocation behavior Deformation mechanisms Critical resolved shear stress

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内蒙古白云鄂博矿床年代学特征及其地质意义

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地质科技通报 2024年第1期43卷 63-73页

作者：陈彪贾晓琪魏威金海龙包头稀土研究院白云鄂博稀土资源研究与综合利用全国重点实验室内蒙古包头014030

内蒙古白云鄂博矿床是世界罕见的特大型REE-Nb-Fe多金属共生矿床,由于经历了复杂的区域地质演化历史,至今仍对稀土成矿时代认识不一。基于前人的同位素年代学研究成果,结合矿床地质特征对稀土成矿时代进行讨论。研究表明,白云鄂博矿区... 详细信息

内蒙古白云鄂博矿床是世界罕见的特大型REE-Nb-Fe多金属共生矿床,由于经历了复杂的区域地质演化历史,至今仍对稀土成矿时代认识不一。基于前人的同位素年代学研究成果,结合矿床地质特征对稀土成矿时代进行讨论。研究表明,白云鄂博矿区经历了华北克拉通2.5~1.8 Ga的前寒武纪构造演化过程;哥伦比亚超大陆裂解的最后阶段,约1.3 Ga在白云鄂博裂谷形成了巨型稀土矿床,与同期碳酸岩墙形成时代一致;受后期华北克拉通北缘古亚洲洋俯冲碰撞造山的影响,白云鄂博地区引发热液交代活动,形成了晚期稀土矿脉和原有稀土矿物的重结晶,导致H 8赋矿白云岩同位素系统受到扰动,呈现出多期次(1.0~0.2 Ga)的同位素年龄结果。总之,白云鄂博是一个在约1.3 Ga裂谷成矿并叠加了加里东和海西2期热扰动事件的巨型稀土矿床。

关键词：白云鄂博矿床同位素年龄稀土成矿时代华北克拉通

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低温高应变量衬板控轧高固溶Al-Mg合金高强塑性与高热稳定性机制

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金属学报 2024年第4期60卷 473-484页

作者：田滕查敏殷皓亮花珍铭贾海龙王慧远吉林大学材料科学与工程学院汽车材料教育部重点实验室长春130025 吉林大学超硬材料国家重点实验室长春130012 吉林大学未来科学国际合作联合实验室长春130012

通过大变形技术制备的高强Al-Mg合金具有广阔应用前景,但其塑性低和高温稳定性差的缺点严重限制其进一步发展。本工作采用低温高应变量衬板控轧(cryogenic high-reduction hard-plate rolling,CHR-HPR)制备了兼具高强塑性(抗拉强度约597... 详细信息

通过大变形技术制备的高强Al-Mg合金具有广阔应用前景,但其塑性低和高温稳定性差的缺点严重限制其进一步发展。本工作采用低温高应变量衬板控轧(cryogenic high-reduction hard-plate rolling,CHR-HPR)制备了兼具高强塑性(抗拉强度约597 MPa、延伸率约7.7%)和高热稳定性的高固溶Mg含量Al-9Mg合金。利用EBSD、TEM、硬度测量和拉伸实验等方法系统研究了Mg含量对CHR-HPR Al-Mg合金微观组织和力学性能的影响。结果表明:CHR-HPR Al-9Mg合金中高含量固溶Mg原子与低温变形促进合金中形成了高密度位错及小角晶界,显著提高合金的屈服强度;高含量固溶Mg原子与可动位错交互作用引起的动态应变时效导致合金加工硬化能力提高,进一步提高了合金的抗拉强度和塑性。此外,在再结晶退火过程中,高含量固溶Mg原子有效地抑制位错滑移、钉扎晶界,延缓回复与再结晶的发生。因此,CHR-HPR Al-Mg合金热稳定性随固溶Mg含量增加而显著提高,其中CHR-HPR Al-9Mg合金再结晶温度达到400℃。

关键词： Al-Mg合金低温衬板控轧加工硬化力学性能微观组织再结晶

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超声引导闭合复位克氏针固定治疗不同类型儿童不稳定型肱骨外髁骨折疗效比较

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中国修复重建外科杂志 2024年第3期38卷 278-283页

作者：刘朝宇贾国强黄秀明申向阳姚杰马海龙安徽医科大学附属阜阳市人民医院骨科安徽阜阳236000 安徽医科大学儿童医学中心合肥230051 赣州市妇幼保健院骨科江西赣州341000

目的探讨超声引导下闭合复位克氏针固定治疗不同类型不稳定型肱骨外髁骨折患儿临床疗效。方法回顾分析2021年1月—2022年10月3个医疗中心收治的94例不稳定型肱骨外髁骨折患儿临床资料。根据Song分型及是否合并关节脱位分为3组,其中Son... 详细信息

目的探讨超声引导下闭合复位克氏针固定治疗不同类型不稳定型肱骨外髁骨折患儿临床疗效。方法回顾分析2021年1月—2022年10月3个医疗中心收治的94例不稳定型肱骨外髁骨折患儿临床资料。根据Song分型及是否合并关节脱位分为3组,其中Song 4型42例(A组)、Song 5型38例(B组)、合并关节脱位14例(C组)。3组患儿性别、年龄、侧别、致伤原因、受伤至手术时间等基线资料比较差异无统计学意义(P>0.05)。均采用超声引导下闭合复位克氏针固定治疗。记录并比较3组患儿手术时间及术后并发症发生情况;采用超声评估闭合复位失败情况。末次随访时行X线片检查,测量患侧Baumann角、髁干角、提携角、外侧骨赘等影像学指标;并测量患侧肘关节伸直、屈曲、旋前、旋后活动度;采用Mayo评分评价肘关节功能。结果 A组手术时间显著多于B、C组,差异均有统计学意义(P0.05)。A、B、C组分别有7、2、5例发生闭合复位失败,失败率比较差异无统计学意义(P>0.05)。患儿均获随访,随访时间6~28个月,平均15.7个月;3组随访时间比较差异无统计学意义(P>0.05)。术后并发症:A组2例延迟愈合,4例针道感染,1例滑车坏死,39例发生外侧骨赘;B组1例畸形愈合,5例针道感染,1例再移位,26例发生外侧骨赘;C组2例针道感染,10例发生外侧骨赘。3组各种并发症发生率比较差异均无统计学意义(P>0.05)。所有患儿均无肘内、外翻畸形发生。末次随访时,除A组髁干角显著大于B、C组(P0.05)。结论超声引导下闭合复位克氏针固定治疗Song 4型肱骨外髁骨折手术时间长、术后并发症多,更易发生外侧骨赘。

关键词：肱骨外髁骨折超声引导闭合复位儿童

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Organocatalytic atroposelective construction of axially chiral nonsymmetric biaryltriols and their applications in asymmetric synthesis and heavy metal ion detection

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Organic Chemistry Frontiers 2022年第4期9卷 923-928页

作者： Shiqi jia Wenling Qin Pengfei Wang hailong Yan Chongqing Key Laboratory of Natural Product Synthesis and Drug Research School of Pharmaceutical SciencesChongqing 401331P.R.China

An organocatalytic methodology toward the atroposelective construction of axially chiral nonsymmetric biaryltriols has been successfully developed.A quinine-derived thiourea-catalyzed intramolecular reaction using VQM(vinylidene ortho-quinone methides)intermediates enabled efficient access to a class of axially chiral nonsymmetric biaryltriols with up to 98%yield and 99%ee.

关键词： chiral symmetric axial

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