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A facile one-pot synthesis of supercubes of Pt nanocubes

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Science China chemistry 2016年第4期59卷 452-458页

作者： Dandan Zang Huaqi Huang Ruixuan Qin Xingli Wang Xiaoliang fang nanfeng zheng state key laboratory for physical chemistry of solid surfaces Collaborative Innovation Center of Chemistry for Energy MaterialsEngineering Research Center for Nano-Preparation Technology of Fujian ProvinceCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Pen-Tung Sah Institute of Micro-Nano Science and Technology Xiamen UniversityXiamen 361005China

A facile one-pot synthetic strategy is developed to prepare high-quality Pt supercubes. The as-synthesized Pt supercubes are composed of the uniform Pt nanocubes arranged in a primitive cubic structure. The shape and size of the Pt superparticles are readily tuned by varying the structures of pyridyl-containing ligands used in the synthesis. The co-presence of CO and nitrogen-containing ligands is critical to the formation of Pt supercubes. While CO molecules play an important role in the synthesis of Pt nanocube, introducing nitrogen-containing ligands is essential to the successful assembly of those nanocubes into Pt supercubes. Our systematic studies reveal that the electrostatic attraction between positively charged ligands and nega- tively charged Pt nanocubes is the main driving force for the assembly of Pt nanocubes into supercubes. More importantly, the ligands within the Pt supercubes are readily removed at relatively low expected to exhibit unique size-selective catalysis. temperature to yield surface-clean supercubes which are

关键词： platinum nanocube supercube self-assembly electrostatic interaction

Pd@Ir-LOD multienzyme utilizing endogenous lactate consumption cooperates with photothermal for tumor therapy

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Nano Research 2024年第1期17卷 270-281页

作者： Zichen Ye Yun Li Jingchao Li Xinyan Hu Jinyang zheng Gongxin Zhang Sijin Xiang Tianbao Zhu Zhide Guo Xiaolan Chen state key laboratory for physical chemistry of solid surfaces Collaborative Innovation Center of Chemistry for Energy Materials and Engineering Research Center for Nano-Preparation Technology of Fujian ProvinceCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China state key laboratory of Molecular Vaccinology and Molecular Diagnostics&Center for Molecular Imaging and Translational Medicine School of Public Health Xiamen UniversityXiamen 361102China The High Educational key laboratory for Biomedical Engineering&key laboratory of fire Retardant Materials of fujian Province Department of BiomaterialsCollege of MaterialsXiamen UniversityXiamen 361102China

Lactic acid(LA)plays a major role in the occurrence,development,and spread of *** by its high accumulation in tumor site,a novel lactate oxidase(LOD)conjugated two-dimensional Pd@Ir nanoplatform(Pd@Ir-LOD,PIL)was fabricated to combine cascade reaction with photothermal for tumor *** detail,the overexpressed LA in tumor microenvironment(TME)was a key factor to activate the PIL-based cascade reaction:(1)Plenty of H_(2)O_(2)could be generated from LA by the catalysis of LOD with O_(2);(2)potent·OH was produced from H_(2)O_(2)due to the peroxidase(POD)-like activity of PIL;(3)meantime,PIL’s catalase(CAT)-like activity could decompose part H_(2)O_(2)into O_(2)to achieve the purpose of LA cyclic ***,the reduced glutathione(GSH)scavenging capability of PIL might protect the produced reactive oxygen species(ROS)from being cleared to further improve the cascade therapeutic *** importantly,PIL had excellent photothermal conversion efficiency(37.35%)and manifested a surprising temperature rising effect in *** together,the decreasing LA concentration,accumulation of high-toxic ROS,the depletion of GSH together with the higher intra-tumoral temperature potently enhanced in vivo antitumor ***,a promising therapeutic tactic based on PIL integrating endogenous LA consumption,chemodynamic therapy(CDT),and photothermal therapy(PTT)has been put forward.

关键词： lactate oxidase chemodynamic therapy photothermal therapy cascade reaction tumor microenvironment

Safety profile of two-dimensional Pd nanosheets for photothermal therapy and photoacoustic imaging

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Nano Research 2017年第4期10卷 1234-1248页

作者： Mei Chen Shuzhen Chen Chengyong He Shiguang Mo Xiaoyong Wang Gang Liu nanfeng zheng state key laboratory for physical chemistry of solid surfaces Collaborative Innovation Center of Chemistry for Energy Materials and Engineering Research Center for Nano-Preparation Technology of Fujian Province College of Chemistry and Chemical Engineering Xiamen University Xiamen 361005 China state key laboratory of Molecular Vaccinology and Molecular Diagnostics Center for Molecular Imaging and Translational Medicine School of Public Health Xiamen University Xiamen 361005 China department of Microbiology and Immunology Xiamen Medical College Xiamen 361008 China

Two-dimensional （2D） nanosheets have emerged as an important class of nanomaterial with great potential in the field of biomedicines, particularly in cancer theranostics. However, owing to the lack of effective methods that synthesize uniform 2D nanomaterials with controlled size, systematic evaluation of size-dependent bio-behaviors of 2D nanomaterials is rarely reported. To the best of our knowledge, we are the first to report a systematic evaluation of the influence of size of 2D nanomaterials on their bio-behaviors. 2D Pd nanosheets with diameters ranging from 5 to 80 nm were synthesized and tested in cell and animal models to assess their size-dependent bioapplication, biodistribution, elimination, toxicity, and genomic gene expression profiles. Our results showed size significantly influences the biological behaviors of Pd nanosheets, including their photothermal and photoacoustic effects, pharmacokinetics, and toxicity. Compared to larger-sized Pd nanosheets, smaller-sized Pd nanosheets exhibited more advanced photoacoustic imaging and photothermal effects upon ultralow laser irradiation. Moreover, in vivo results indicated that 5-nm Pd nanosheets escape from the reticuloendothelial system with a longer blood half-life and can be cleared by renal excretion, while Pd nanosheets with larger sizes mainly accumulate in the liver and spleen. The 30-nm Pd nanosheets exhibited the highest tumor accumulation. Although Pd nanosheets did not cause any appreciable toxicity at the cellular level, we observed slight lipid accumulation in the liver and inflammation in the spleen. Genomic gene expression analysis showed that 80-nm Pd nanosheets interacted with more cellular components and affected more biological processes in the liver, as compared to 5-nm Pd nanosheets. We believe this work will provide valuable information and insights into the clinical application of 2D Pd nanosheets as nanomedicines.

关键词： Pd nanosheets photothermal therapy photoacoustic imaging toxicity evaluation genomic gene expression

Air-promoted selective hydrogenation of phenol to cyclohexanone at low temperature over Pd-based nanocatalysts

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Science China chemistry 2017年第11期60卷 1444-1449页

作者： Qing Guo Shiguang Mo Pengxin Liu Weidong zheng Ruixuan Qin Chaofa Xu Youyunqi Wu Binghui Wu nanfeng zheng department of Chemical and Biochemical Engineering National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-EstersState Key Laboratory for Physical Chemistry of Solid SurfacesCollaborative Innovation Center of Chemistryfor Energy Materialsand Engineering Research Center for Nano-Preparation Technology of Fujian ProvinceCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China

Attaining high activity with high selectivity at low temperature is challenging in the selective hydrogenation of phenol to cyclohexanone due to its high activation energy （Ea, 55-70 kJ/mol）. Here we report a simple and efficient strategy for phenol hydrogenation catalyzed by Pd in aqueous phase at 30 ℃ by introducing air to promote the catalysis. With the assistance of air, 〉99% conversion and 〉99% selectivity were achieved over Pd（111）/Al2O3 with an overall turnover frequency （TOf） of 621 h-1, -80 times greater than that of the state-of-art Pd catalyst at 30 ℃. Mechanism studies revealed that phenol was activated to generate phenoxyl radicals. The radicals were yielded from the reaction between phenol and hydroxyl radicals in the presence of hydrogen, oxygen and protic solvent on Pd. The phenoxyl pathway resulted in a low apparent Ea （8.2 kJ/mol） and thus high activity. More importantly, this strategy of activating substrate by air can be adapted to other Pd based catalysts, offering a new thinking for the rational design of cyclohexanone production in industry.

关键词： selective hydrogenation phenol palladium nanocatalysis radical

A vicinal effect for promoting catalysis of Pd1/TiO2:supports of atomically dispersed catalysts play more roles than simply serving as ligands

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Science Bulletin 2018年第11期63卷 675-682页

作者： Pengxin Liu Yun Zhao Ruixuan Qin Lin Gu Peng Zhang Gang fu nanfeng zheng Collaborative Innovation Center of chemistry for Energy Materials.state key laboratory for physical chemistry of solid surfaces Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Institute of Physics Chinese Academy of SciencesBeijing 100190China department of chemistry Dalhousie UniversityHalifaxNS B3H4R2Canada

Atomically dispersing metal atoms on supports has been emerging as an effective strategy to maximize the atom utilization of metals for catalysis. However, due to the lack of effective tools to characterize the detailed structure of metal-support interface, the chemical functions of supports in atomically dispersed metal catalysts are hardly elucidated at the molecular level. In this work, an atomically dispersed Pdl/ Ti02 catalyst with Ti（III） vicinal to Pd is prepared and used to demonstrate the direct involvement of metal atoms on support in the catalysis of dispersed metal atoms. Systematic studies reveal that the Ti （IlI）-O-Pd interface facilitates the activation of 02 into superoxide （02）, thus promoting the catalytic oxi- dation. The catalyst exhibits the highest CO turn-over frequency among ever-reported Pd-based catalysts, and enhanced catalysis in the combustion of harmful volatile organic compound （i.e., toluene） and green- house gas （i.e., methane）. The demonstrated direct involvement of metal atoms on oxide support suggests that the real active sites of atomically dispersed metal catalysts can be far beyond isolated metal atoms themselves. Metal atoms on oxide supports in the vicinity serve as another vector to promote the catalysis of atomically dispersed metal catalysts.

关键词： Support effect Ligand effect Single-atom catalyst Oxidation reaction Superoxide

Effect of glutathione on in vivo biodistribution and clearance of surface-modified small Pd nanosheets

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Science China chemistry 2015年第11期58卷 1753-1758页

作者： Yizhuan Huang Xiaolan Chen Saige Shi Mei Chen Shaoheng Tang Shiguang Mo Jingping Wei nanfeng zheng state key laboratory for physical chemistry of solid surfaces department of chemistry College of Chemistry and Chemical EngineeringXiamen University

Plasmonic Pd nanosheets have been emerging as promising materials for application in near-infrared(NIR) photothermal therapy(PTT) of cancer. However, animal in mice studies indicated that the original synthesized poly(vinylpyrrolidone)(PVP)-protected small Pd nanosheets(Pd-PVP) and some further surface-modified small Pd nanosheets such as Pd-PEG(SH) easily accumulated in reticuloendothelial system(RES) organs(liver, spleen, etc.) and were difficult to be cleared from these organs quickly. In the work, we surprisingly found that glutathione(GSH) could promote the clearance of surface-modified small Pd nanosheets(e.g. Pd-PVP, Pd-PEG(SH) and Pd-GSH) from the RES organs efficiently. The effects of GSH on the biodistribution and clearance of different surface-modified Pd nanosheets were investigated. Our results indicated that these surface-modified Pd nanosheets with or without GSH added caused no morbidity at target primary organs, and GSH can promote the clearance of different surface-modified Pd nanosheets in the order of Pd-PVP≈Pd-PEG(SH)>Pd-GSH. This study suggests that glutathione could be an attractive reagent for promoting nanomaterials eliminated from the reticuloendothelial systems(RES).

关键词： noble metal nanomaterials glutathione biodistribution renal clearance

Dynamic tracking of exsolved PdPt alloy/perovskite catalyst for efficient lean methane oxidation

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Chinese Chemical Letters 2024年第4期35卷 170-175页

作者： Yanling Yang Zhenfa Ding Huimin Wang Jianhui Li Yanping zheng Hongquan Guo Li Zhang Bing Yang Qingqing Gu Haifeng Xiong Yifei Sun College of Energy Xiamen UniversityXiamen 361005China School of Environment and Civil Engineering Dongguan University of TechnologyDongguan 523808China department of chemistry College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China state key laboratory of physical chemistry of solid surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China CAS key laboratory of Science and Technology on Applied Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China Innovation laboratory for Sciences and Technologies of Energy Materials of fujian Province(IKKEM) Xiamen 361102China

Supported Pd based catalysts are considered as the efficient candidates for low-carbon alkane oxidation for their outstanding capability to break C-H bond. Whereas, the irreversible deactivation of Pd based catalysts was still frequently observed. Herein, we reinforced the extruded Pd nanoparticles with quantitive Pt to assemble the evenly distributed Pd Pt nanoalloy onto ferrite perovskite(Pd Pt-LCf) matrix with strengthened robustness of metal/oxide support interface. We further co-achieved the enhanced performance, anti-overoxidation as well as resistance of vapor-poisoning in durability measurement. The operando X-ray photoelectron spectroscopy(O-XPS) combined with various morphology characterizations confirms that the accumulation of surface deep-oxidation species of Pd^(4+) is the culprit for fast activity loss in exsolved Pd system, especially at high temperature of 400 ℃. Conversely, it could be completely suppressed by in-situ alloying Pd with equal amount of Pt, which helps maintain the metastable Pd^(2+)/Pd shell and metallic solid-solution core structure. The density function theory(DfT) calculations further buttress that the dissociation of C–H was facilitated on alloy/perovskite interface which is, on the contrary, resistant toward O–H bond cleavage, as compared to Pd/perovskite. Our work suggests that the modification of exsolved metal/oxide catalytic interface could further enrich the toolkit of heterogeneous catalyst design.

关键词： Exsolution PdPt alloy Operando characterization Methane conversion Deep-oxidation

Antioxidant high-conductivity copper paste for low-cost flexible printed electronics

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npj flexible Electronics 2022年第1期6卷 176-184页

作者： Shuqing Hong Chimin Liu Shuqiang Hao Wenxing fu Jian Peng Binghui Wu nanfeng zheng Pen-Tung Sah Institute of Micro-Nano Science and Technology State Key Laboratory for Physical Chemistry of Solid SurfacesCollaborative Innovation Center of Chemistry for Energy MaterialsNational&Local Joint Engineering Research Center of Preparation Technology of NanomaterialsCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Innovation laboratory for Sciences and Technologies of Energy Materials of fujian Province(IKKEM) Xiamen 361005China

The flexible printed electronics(e.g.,wearable devices,roll-up displays,heating circuits,radio frequency identification(RfID)tags)calls for high-conductivity and low-cost materials,particularly for copper *** is still a big challenge to develop reliable copper pastes for both antioxidant and high-conductivity flexible printed films and *** this work,an antioxidant copper paste was achieved using copper microflakes with surface passivation by formate ions and thiols,with high conductivity of 13400 S cm^(−1)(the same order of magnitude of silver pastes,1.8-2.5×10^(4) S cm^(−1)).The universal applications of as-prepared copper paste in flexible printed electronics(e.g.,electromagnetic interference(EMI)shielding films,anti-fog films,and RfID tags)via screen printing and curing at 170℃ under ambient atmosphere were *** as-printed electronics showed high performance in flexibility,stability,and *** work shows the great potential of anti-oxidation copper pastes in low-cost flexible printed electronics for commercial usage.

关键词： paste copper cost

Superatomic Aub clusters ligated by different N-heterocyclic carbenes and their ligand-dependent catalysis, photoluminescence, and proton sensitivity

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Nano Research 2020年第7期13卷 1908-1911页

作者： Hui Shen Sijin Xiang Zhen Xu Chen Liu Xihua Li Cunfa Sun Shuichao Lin Boon K.Teo nanfeng zheng state key laboratory for physical chemistry of solid surfaces Collaborative Innovation Center of Chemistry for Energy MaterialsNational&Local Joint Engineering Research Center of Preparation Technology of NanomaterialsCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China School of Pharmaceutical Science Xiamen UniversityXiamen 361002China

We report herein a class of superatomic AU13 clusters stabilized by different N-heterocyclic carbenes(NHCs).The clusters show diverse metal surface structures,properties and functions as exemplified by:(1)the first anionic AU13 cluster[Au1g(NHC-1)sBr6],which has bulky NHC-1 ligands that lead to a rather open metal surface contributing to its high catalytic activity;(2)the tricationic cluster[Au13(NHC-2)sBr2]+which has bidentate,benzyl-rich NHC-2 ligands that make it ultra-stable and highly-luminescent,suitable for bio-imaging;and(3)by bearing two pyridyl groups on NHC-3,the dicationic cluster[Au:a(NHC-3)gClg]f+exhibits reversible and stable visible absorption and solubility responses to protonation/deprotonation cycles,making it a potential pH sensor(NHC-1=1,3-disopropylbenzimidazolin-ylidene;NHC-2=1,3-bis(1-benzyl-1H-benzimidazol-1-ium-yl)propane;NHC-3=1,3-bis(icolyI)benzimidazolin-ylidene).The study nicely demonstrates the importance of ligands in designing metal nanoclusters with desired functionalities.

关键词： carbene ligands gold nanocluster catalysis luminescenee Au13