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Electronic properties and photodegradation ability of Nd-TiO_(2)for phenol

Journal of Rare Earths 2022年第7期40卷 1063-1072页

作者： Zhimin Zhao jinjia liu Gala Sa Aiju Xu Inner Mongolia Key Laboratory of Green Catalysis College of Chemistry and Environmental ScienceInner Mongolia Normal UniversityHohhot 010022China State Key Laboratory of Coal Conversion Institute of Coal Chemistry Chinese Academy of SciencesTaiyuan 030001China National Energy Center for Coal to Clean Fuels Synfuels China Co.Ltd.Beijing 101400China

In this study,the photocatalytic activity of Nd-TiO_(2)photocatalysts obtained by common hydrothermal method was evaluated by practical experiments and theoretical calculations based on density functional theory(DFT).The synthesized photocatalysts were characterized by X-ray diffraction(XRD),N_(2)adsorption-desorption,Fourier transform infrared spectroscopy(FT-IR),high resolution transmission electron microscopy(HRTEM),X-ray photoelectron spectroscopy(XPS),UV-Vis diffuse reflectance spectroscopy(DRS),and photoluminescence(PL)to study their physical/chemical prope rties.At the same time,the photoelectronic performance was also investigated.The photodegradation ability of asprepared photocatalysts and the effect of Nd doped amount and photocatalysts dosage were investigated by the photodegradation of phenol(30 mg/L)under 400 W metal halide lamp(UV-Vis).The effect of Nd on electronic properties of TiO_(2)and adsorption ability of phenol were discussed.Results show the red-shift wavelength of 0.5 mol%Nd-TiO_(2),indicating that its absorption capacity is stronger than pristine TiO_(2)in the same wavelength range.The result of DFT calculations demonstrates that the optical bandgap of Nd-TiO_(2)is profoundly reduced,thus the light absorption ability is promoted,which will be responsible for the enhanced photocatalytic performance of Nd-TiO_(2).0.5 mol%Nd is an optimum value for photodegradation phenol,and phenol can be completely degraded by 0.5 mol%Nd-TiO_(2)for 210 min,the higher catalytic performance is derived from the efficient separation of e-/h+pairs.Moreover,the adsorption energy calculations of phenol on TiO_(2)(101)and Nd-TiO_(2)(101)demonstrate that the Nd doping can significantly enhance the adsorption ability of phenol on catalyst surfaces because of the formation of Nd-O bonds.At last,the stability measurement through four recycles exhibits that 0.5 mol%Nd-TiO_(2)possesses excellent stability.

关键词： TiO_(2) Hydrothermal method Density functional theory Phenol Photodegradation Rare earths

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Theoretical study on the morphology of cobalt nanoparticles modulated by alkali metal promoters

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矿物冶金与材料学报:英文版 2023年第10期30卷 2006-2013页

作者： Xiaobin Geng Hui Yang Wenping Guo Xiaotong liu Tao Yang jinjia liu National Energy Center for Coal to Liquids Synfuels China Co.LtdBeijing 101400China State Key Laboratory of Coal Conversion Institute of Coal ChemistryChinese Academy of SciencesTaiyuan 030001China University of Chinese Academy of Sciences Beijing 100049China Beijing Advanced Innovation Center for Materials Genome Engineering Beijing Information Science and Technology UniversityBeijing 100101China School of Computer Beijing Information Science and Technology UniversityBeijing 100101China College of Chemistry and Environmental Science Inner Mongolia Key Laboratory of Green CatalysisInner Mongolia Normal UniversityHohhot 010022China

Cobalt nanoparticles(NPs)catalysts are extensively used in heterogeneous catalytic reactions,and the addition of alkali metal promoters is a common method to modulate the catalytic performance because the catalyst's surface structures and morphologies are sensitive to the addition of promoters.However,the underlying modulation trend remains unclear.Herein,the adsorption of alkali metal promoters(Na and K)on the surfaces of face-centered-cubic(FCC)and hexagonal-closest packed(HCP)polymorphous cobalt was systematically investigated using density functional theory.Furthermore,the effect of alkali promoters on surface energies and nanoparticle morphologies was revealed on the basis of Wulff theory.For FCC-Co,the exposed area of the(111)facet in the nanoparticle increases with the adsorption coverage of alkali metal oxide.Meanwhile,the(311),(110),and(100)facets would disappear under the higher adsorption coverage of alkali metals.For HCPCo,the Wulff morphology is dominated by the(0001)and(1011)facets and is independent of the alkali metal adsorption coverage.This work provides insights into morphology modulation by alkali metal promoters for the rational design and synthesis of cobalt-based nanomaterials with desired facets and morphologies.

关键词： cobalt nanoparticles alkali promoter density functional theory crystal morphology Wulff construction

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Self-adjuvant Astragalus polysaccharide-based nanovaccines for enhanced tumor immunotherapy:a novel delivery system candidate for tumor vaccines

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Science China(Life Sciences) 2024年第4期67卷 680-697页

作者： Nan Li Yun Zhang Miaomiao Han Tian liu jinjia Wu Yingxia Xiong Yikai Fan Fan Ye Bing Jin Yinghua Zhang Guibo Sun Xiaobo Sun Zhengqi Dong State Key Laboratory for Quality Ensurance and Sustainable Use of Dao-di Herbs Chinese Academy of Medical Sciences&Peking Union Medical College(CAMS)Institute of Medicinal Plant Development(IMPLAD)Beijing 100193China Key Laboratory of Bioactive Substances and Resources Utilization of Chinese Herbal Medicine from Ministry of Education Beijing Key Laboratory of Innovative Drug Discovery of Traditional Chinese Medicine(Natural Medicine)and Translational MedicineKey Laboratory of New Drug Discovery Based on Classic Chinese Medicine Prescription from Chinese Academy of Medical SciencesCAMSIMPLADBeijing 100193China Department of Pharmaceutics School of Pharmaceutical SciencesHeilongjiang University of Chinese MedicineHarbin 150036China Jilin Academy of Chinese Medicine Sciences Changchun 130012China Joint Research Center for Chinese Medicinal Herbs IMPLADABRC&ACCLBeijing 100193China

The study of tumor nanovaccines(NVs)has gained interest because they specifically recognize and eliminate tumor cells.However,the poor recognition and internalization by dendritic cells(DCs)and insufficient immunogenicity restricted the vaccine efficacy.Herein,we extracted two molecular-weight Astragalus polysaccharides(APS,12.19 k D;APSHMw,135.67 k D)from Radix Astragali and made them self-assemble with OVA257–264directly forming OVA/APS integrated nanocomplexes through the microfluidic method.The nanocomplexes were wrapped with a sheddable calcium phosphate layer to improve stability.APS in the formed nanocomplexes served as drug carriers and immune adjuvants for potent tumor immunotherapy.The optimal APS-NVs were approximately 160 nm with uniform size distribution and could remain stable in physiological saline solution.The FITC-OVA in APS-NVs could be effectively taken up by DCs,and APS-NVs could stimulate the maturation of DCs,improving the antigen cross-presentation efficiency in vitro.The possible mechanism was that APS can induce DC activation via multiple receptors such as dectin-1 and Toll-like receptors 2 and 4.Enhanced accumulation of APS-NVs both in draining and distal lymph nodes were observed following s.***.injection.Smaller APS-NVs could easily access the lymph nodes.Furthermore,APS-NVs could markedly promote antigen delivery efficiency to DCs and activate cytotoxic T cells.In addition,APS-NVs achieve a better antitumor effect in established B16-OVA melanoma tumors compared with the OVA+Alum treatment group.The antitumor mechanism correlated with the increase in cytotoxic T cells in the tumor region.Subsequently,the poor tumor inhibitory effect of APS-NVs on the nude mouse model of melanoma also confirmed the participation of antitumor adaptive immune response induced by NVs.Therefore,this study developed a promising APS-based tumor NV that is an efficient tumor immunotherapy without systemic side effects.

关键词： Astragalus polysaccharides nanovaccines OVA immunotherapy self-adjuvant

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Fecal metabolomics reveals the positive effect of ethanol extract of propolis on T2DM mice

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Food Science and Human Wellness 2023年第1期12卷 161-172页

作者： Chunmei Wang Huiting Zhao Kai Xu Yali Du jinjia liu Jinfei Wang Yusuo Jiang College of Animal Science Shanxi Agricultural UniversityTaigu 030801China College of Life Sciences Shanxi Agricultural UniversityTaigu 030801China Jilin Province Institute of Apicultural Science Jilin 132108China College of Veterinary Medicine Shanxi Agricultural UniversityTaigu 030801China

A large number of studies have shown that propolis has positive effects in the treatment of type 2 diabetes mellitus(T2DM).However,there are have only been a few reports that are based on an ultra-high performance liquid chromatography-quadrupole-time-of-flight-mass spectrometry(UPLC-Q-TOF-MS)analysis of the fecal metabolomics of ethanol extract of propolis(EEP)in the treatment of T2DM.The present investigation was designed to screen potential biomarkers of T2DM by the metabonomic method and to explain the possible anti-diabetes mechanism of EEP according to the changes in the biomarkers.The results showed that EEP improved the body weight(BW)of T2DM mice,lowered blood sugar levels,and significantly restored blood biochemical indicators related to T2DM,such as fasting insulin(FINS),homeostasis model assessment of insulin resistance(HOMA-IR),aspartate transaminase(AST),and alanine aminotransferase(ALT).Liver pathology showed that EEP reversed liver damage caused by T2DM.Metabolomics data identified 27 potential biomarkers in fecal samples.EEP effectively regulated the dysfunction in the metabolic pathways of glycerophospholipids,sphingolipids,riboflavins,and sterol lipids caused by T2DM.In summary,our research results revealed positive effects of EEP in the treatment of T2DM and provided potential candidate markers for further research and in the clinical treatment of T2DM.

关键词： Ethanol extract of propolis Type 2 diabetes mellitus Fecal metabolites UPLC-Q-TOF-MS Metabolomics

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Speeding up the prediction of C-O cleavage through bond valence and charge on iron carbides

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矿物冶金与材料学报:英文版 2023年第10期30卷 2014-2024页

作者： Yurong He Kuan Lu jinjia liu Xinhua Gao Xiaotong liu Yongwang Li Chunfang Huo James P.Lewis Xiaodong Wen Ning Li Beijing Advanced Innovation Center for Materials Genome Engineering Beijing Information Science&Technology UniversityBeijing 101400China State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering College of Chemistry and Chemical EngineeringNingxia UniversityYinchuan 750021China State Key Laboratory of Coal Conversion Institute of Coal ChemistryChinese Academy of SciencesTaiyuan 030001China National Energy Center for Coal to Liquids Synfuels China Co.Ltd.Beijing 101400China Hong Kong Quantum AI Laboratory Ltd.University of Hong KongHong Kong 999077China

The activation of CO on iron-based materials is a key elementary reaction for many chemical processes.We investigate CO adsorption and dissociation on a series of Fe,Fe_(3)C,Fe_(5)C_(2),and Fe_(2)C catalysts through density functional theory calculations.We detect dramatically different performances for CO adsorption and activation on diverse surfaces and sites.The activation of CO is dependent on the local coordination of the molecule to the surface and on the bulk phase of the underlying catalyst.The bulk properties and the different local bonding environments lead to varying interactions between the adsorbed CO and the surface and thus yielding different activation levels of the C-O bond.We also examine the prediction of CO adsorption on different types of Fe-based catalysts by machine learning through linear regression models.We combine the features originating from surfaces and bulk phases to enhance the prediction of the activation energies and perform eight different linear regressions utilizing the feature engineering of polynomial representations.Among them,a ridge linear regression model with2nd-degree polynomial feature generation predicted the best CO activation energy with a mean absolute error of 0.269 eV.

关键词： adsorption CO activation iron carbides density functional theory

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Atomically dispersed Zn-Co-N-C catalyst boosting efficient and robust oxygen reduction catalysis in acid via stabilizing Co-N bonds

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Fundamental Research 2023年第6期3卷 909-917页

作者： Feng Ma Xuan liu Xiaoming Wang Jiashun Liang Jianyu Huang Cameron Priest jinjia liu Shuhong Jiao Tanyuan Wang Gang Wu Yunhui Huang Qing Li State Key Laboratory of Material Processing and Die&Mould Technology School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhanHubei 430074China State Key Laboratory of Refractories and Metallurgy Institute of Advanced Materials and NanotechnologyKey Laboratory of Hubei Province for Coal Conversion and New Carbon MaterialsSchool of Chemistry and Chemical EngineeringWuhan University of Science and TechnologyWuhan 430081China Clean Nano Energy Center State Key Laboratory of Metastable Materials Science and TechnologyYanshan UniversityQinhuangdao 066004China Department of Chemical and Biological Engineering University at BuffaloThe State University of New YorkBuffaloNY 14260United States State Key Laboratory of Coal Conversion Institute of Coal ChemistryChinese Academy of SciencesTaiyuan 030001China National Energy Center for Coal to Clean Fuels Synfuels China Co.LtdHuairou DistrictBeijing 101400China Department of Materials Science and Engineering Key Laboratory of Materials for Energy Conversion Chinese Academy of Science(CAS)University of Science and Technology of ChinaHefei 230026China Department of Chemistry and Key Laboratory for Preparation and Application of Ordered Structural Materials of Guangdong Province Shantou UniversityShantou 515063China

Transition metal supported N-doped carbon(M-N-C)catalysts for oxygen reduction reaction(ORR)are viewed as the promising candidate to replace Pt-group metal(PGM)for proton exchange membrane fuel cells(PEMFCs).However,the stability of M-N-C is extremely challenging due to the demetalation,H_(2)O_(2)attack,etc.in the strongly oxidative conditions of PEMFCs.In this study,we demonstrate the universal effect of Zn on promoting the stability of atomically dispersed M-Nx/C(M=Co,Fe,Mn)catalysts and the enhancement mechanism is unveiled for the first time.The best-performing dual-metal-site Zn-Co-N-C catalyst exhibits a high half-wave potential(E1/2)value of 0.81 V vs.reversible hydrogen electrode(RHE)in acid and outstanding durability with no activity decay after 15,000 accelerated degradation test(ADT)cycles at 60℃,surpassing most reported Co-based PGM-free catalysts in acid media.For comparison,the Co-N-C in the absence of Zn suffers from a rapid degradation after ADT due to the demetalation and higher H_(2)O_(2)yield.X-ray adsorption spectroscopy(XAS)and density functional theory(DFT)calculations suggest the more negative formation energy(by 1.2 eV)and increased charge transfer of Zn-Co dual-site structure compared to Co-N-C could strength the Co-N bonds against the demetalation and the optimized d-band center accounts for the improved ORR kinetics.

关键词： Electrocatalysis Oxygen reduction reaction Non-noble metal catalysts Metal-nitrogen carbon catalysts Demetalation Structural stability

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Molybdenum-doped ordered L1_(0)-PdZn nanosheets for enhanced oxygen reduction electrocatalysis

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SusMat 2022年第3期2卷 347-356页

作者： Jiashun Liang Yu Xia Xuan liu Fanyang Huang jinjia liu Shenzhou Li Tanyuan Wang Shuhong Jiao Ruiguo Cao Jiantao Han Hsing-Lin Wang Qing Li State Key Laboratory of Material Processing and Die and Mould Technology School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhanChina Department of Materials Science and Engineering Southern University of Science and TechnologyShenzhenChina School of Physics and Astronomy University of BirminghamBirminghamUK Key Laboratory of Materials for Energy Conversion Chinese Academy of Science(CAS) Department of Materials Science and EngineeringUniversity of Science and Technology of ChinaHefeiChina Institute of Coal Chemistry Chinese Academy of SciencesTaiyuanChina National Energy Center for Coal to Clean Fuels Synfuels China Co.LtdBeijingChina

Ultrathin Pd-based two-dimensional(2D)nanosheets(NSs)with tunable physicochemical properties have emerged as promising candidate for oxygen reduction reaction(ORR).Unfortunately,structurally ordered Pd-based NSs can be hardly prepared as high temperature annealing(>600℃)is necessary for disorder to order phase transition,making it a considerable challenge for morphology control.Herein,a new class of ultrathin structurally ordered Mo-doped L1_(0)-PdZn NSs with curved geometry and abundant defects/lattice distortions is reported as an efficient oxygen reduction electrocatalyst in alkaline solution.It is found that Mo(CO)_(6) serves as reducing agent and Mo source to generate the unique ordered 2D morphology,which leads to the significantly modified electronic structure.The developed L1_(0)-Mo-PdZn NSs exhibit excellent ORR mass activity of 2.6 A mg_(Pd)^(−1) at 0.9 V versus reversible hydrogen electrode,31.5 and 17.6 times higher than those of Pd/C and Pt/C,respectively,outperforming most of the reported Pdbased ORR electrocatalsyts.Impressively,L1_(0)-Mo-PdZn NSs is extremely stable for ORR,with only 2.3% activity loss after 10000 potential cycles.Density functional theory study suggests that ordered L1_(0) structure and Mo doping can raise the vacancy formation energy of Pd atom and thus promote the ORR stability.

关键词： electrocatalysis fuel cell nanosheeets oxygen reduction Pd-based intermetallics

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Structural and electronic effects boosting Ni-doped Mo_(2)C catalyst toward high-efficiency C-O/C-C bonds cleavage

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Journal of Energy Chemistry 2022年第12期75卷 109-116,I0004页

作者： Xiangze Du jinjia liu Dan Li Hui Xin Xiaomei Lei Rui Zhang Linyuan Zhou Huiru Yang Yan Zeng Hualong Zhang Wentao Zheng Xiaodong Wen Changwei Hu Key Laboratory of Green Chemistry and Technology College of ChemistrySichuan UniversityChengdu 610064SichuanChina State Key Laboratory of Coal Conversion Institute of Coal ChemistryChinese Academy of SciencesTaiyuan 030001ShanxiChina National Energy Center for Coal to Liquids Synfuels China Co.LtdBeijing 101400China Department State Key Laboratory of Catalysis iChEMDalian Institute of Chemical PhysicsChinese Academy of ScienceDalian 116023LiaoningChina Department of Chemistry University of HelsinkiA.I.Virtasen Aukio 1P.O.Box 5500014Finland

The selective cleavage of C-O and C-C is facing a challenge in the field of catalysis.In the present work,we studied the influence of doped Ni on the structure and electronic properties,as well as the selective C-O/C-C bond cleavages in the hydrodeoxygenation of palmitic acid over Ni-Mo_(2)C catalyst.The catalytic activity on Ni doped Mo_(2)C with TOF of 6.9×10^(3)h^(-1)is much superior to intrinsic Mo_(2)C catalyst,which is also higher than most noble metal catalysts.Structurally,the doped Ni raises the active particle dispersion and the coordination numbers of Mo species(Mo-C and Mo-O),improves the graphitization degree to promote the electron transfer,and increases the amount of Lewis and Br?nsted acid,which are responsible for the excellent hydrodeoxygenation performance.The Ni promotes simultaneously C-O and C-C bonds cleavage to produce pentadecane and hexadecane owing to the increase of electron-rich Mo sites after Ni doping.These findings contribute to the understanding of the nature of Ni-doped Mo_(2)C on the roles as catalytic active sites for C-O and C-C bonds cleavage.

关键词： Ni-doped Mo_(2)C Palmitic acid Hydrodeoxygenation C-O/C-C bond cleavages Biofuel

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商周铜器蛇噬蛙纹研究

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辽宁师范大学学报（社会科学版） 2024年第2期47卷 15-21页

作者：张德良刘晋嘉辽宁师范大学历史文化学院辽宁大连116081

搜集饰有蛇噬蛙纹的商周青铜器,计有9件;根据发现地点和纹饰风格,对这些器物做了分区研究,计有东北、北方、西南和南方四个文化区。根据器物所属考古学文化区,发现东北区与北方区为蛇噬蛙纹主要分布区,二区内的蛇噬蛙纹在表现风格上既... 详细信息

搜集饰有蛇噬蛙纹的商周青铜器,计有9件;根据发现地点和纹饰风格,对这些器物做了分区研究,计有东北、北方、西南和南方四个文化区。根据器物所属考古学文化区,发现东北区与北方区为蛇噬蛙纹主要分布区,二区内的蛇噬蛙纹在表现风格上既有联系亦有区别;西南区与南方区的蛇噬蛙纹出现时间相对较晚。追溯这一纹饰母题,据目前所知,兴隆洼文化查海遗址出土的斜腹罐所饰的蛇噬蛙纹当为其源头。

关键词：蛇衔蛙纹青铜器商周文化区

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应用于新型环路热管的两相引射器数值模拟

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化工学报 2024年第1期75卷 268-278页

作者：周尧杨小平倪一程刘继平魏进家严俊杰西安交通大学热流科学与工程教育部重点实验室陕西西安710049 西安交通大学化学工程与技术学院陕西西安710049 西安交通大学动力工程多相流国家重点实验室陕西西安710049

环路热管是一种高效被动式相变传热装置,广泛应用于高热流电子器件散热等领域。前期研究发现将小型两相引射器与平板式环路热管耦合,可大幅提高传热性能。然而,小型两相引射器内部流动及传热机理尚不清晰,难以对新型环路热管进行正向设... 详细信息

环路热管是一种高效被动式相变传热装置,广泛应用于高热流电子器件散热等领域。前期研究发现将小型两相引射器与平板式环路热管耦合,可大幅提高传热性能。然而,小型两相引射器内部流动及传热机理尚不清晰,难以对新型环路热管进行正向设计与理论建模。通过数值模拟研究了汽水参数和混合腔结构对两相引射器性能及内部流场分布的影响。结果表明,喉部下游存在凝结激波,随着背压增加,其位置逐渐向喉部移动;其强度与背压、蒸汽产量、混合腔长度呈正相关,与水温呈负相关。引射器最大工作背压在40~125 kPa,与蒸汽产量和水温呈正相关,与混合腔长度呈负相关。通过大量模拟,得到了设计功率下水温和混合腔长度对引射器工作模式和压比的影响规律。

关键词：环路热管引射器传热两相流凝结激波数值模拟

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