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Synergistic combination of Pd nanosheets and porous Bi(OH)_(3) boosts activity and durability for ethanol oxidation reaction

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Nano Research 2022年第5期15卷 3920-3926页

作者： Mingyu Chu Jialu Huang Jin Gong Yi Qu Guoling Chen Hu Yang Xuchun Wang Qixuan Zhong Chengwei Deng Muhan Cao Jinxing Chen Xiaolei Yuan Qiao Zhang School of Chemistry and Chemical Engineering Nantong University9 Seyuan RoadNantong 226019China Institute of Functional Nano&Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials and DevicesSoochow UniversityNo.199 Ren’ai RoadSuzhou 215123China Department of Chemistry University of Western OntarioLondonOntario N6A5B7Canada State Key Laboratory of Space Power-sources Technology Shanghai Institute of Space Power-Sources2965 Dongchuan RoadShanghai 200245China

Highly active and durable pd-based electrocatalysts for ethanol oxidation reaction(EOR)play a crucial role in the commercialization of direct ethanol fuel cells(DEFCs).However,the poisonous intermediates(especially adsorbed CO species(COad))formed during the EOR process can easily adsorb and block the active sites on pd electrodes,which in turn limits the catalytic efficiency.Hence,we present a series of pd-based composites with a strong coupling interface consisting of Pd nanosheets and amorphous Bi(OH)_(3)species.The incorporation of Bi(OH)3 can induce an electron-rich state adjacent to the pd sites and effectively separate the pd ensemble,leading to excellent CO tolerance.The optimal pd-Bi(OH)_(3)NSs catalyst manifests a mass activity of 2.2 A·mgpd^(-1),which is 5.7 and 2.0 times higher than that of pd NSs and commercial pd/C catalyst,respectively.Further CO-stripping experiments and CO-DRIFTS tests confirm the excellent CO tolerance on pd-Bi(OH)3 NSs electrode,leading to the enhanced EOR durability.

关键词： Pd nanosheets Bi(OH)_(3)species ethanol oxidation reaction Co tolerance

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Enhanced oxidase-like activity of g-C_(3)N_(4) nanosheets supported Pd nanosheets for ratiometric fluorescence detection of acetylcholinesterase activity and its inhibitor

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Chinese Chemical Letters 2022年第2期33卷 757-761页

作者： Chenghui Zhang Pengjuan Ni Bo Wang Wendong Liu Yuanyuan Jiang Chuanxia Chen Jian Sun Yizhong Lu School of Materials Science and Engineering University of JinanJi’nan 250022China State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

The undesirable enzymatic activity of nanozymes under near neutral p H condition and the traditional single signal output always restrict the analytical application of nanozyme-based biosensors.Herein,graphitic carbon nitride nanosheets supported palladium nanosheets composite (pd/g-C_(3)N_(4)) with both oxidase-like activity and fluorescent property is synthesized.Notably,pd/g-C_(3)N_(4)exhibits enhanced oxidase-like activity compared to pd NSs under p H 7.4.By combining pd/g-C_(3)N_(4)with o-phenylenediamine(Opd),a ratiometric fluorescence assay for acetylcholinesterase (ACh E) activity detection is developed.pd/g-C_(3)N_(4)can catalyze oxidation of nonfluorescent Opd to fluorescent oxidized Opd (ox Opd,Em=565nm),which can quench fluorescence of g-C_(3)N_(4)supporter (Em=441 nm) through fluorescence resonance energy transfer (FRET).However,in presence of ACh E,acetylthiocholine can be hydrolyzed into thiocholine,which will block the oxidase-like activity of pd/g-C_(3)N_(4)and then hamper the FRET process.This ratiometric fluorescence assay is also viable to screen ACh E inhibitor.This work will guide design of ratiometric fluorescence assay based on nanozymes with improved enzymatic activity.

关键词： Oxidase-like activity Ratiometric fluorescence Acetylcholinesterase g-C_(3)N_(4)nanosheets Pd nanosheets

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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

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