基于三金属Au@PdPt纳米颗粒修饰花状MnO_(2)纳米片的无标记电化学免疫传感器应用于NT-proBNP的高灵敏度检测

N-末端脑利钠肽前体(NT-proBNP)的灵敏检测是降低心力衰竭死亡率的重要先决条件。在这项研究中,开发了一种无标记电流免疫传感器来灵敏地检测NT-proBNP。它基于三金属Au@PdPt纳米颗粒修饰花状MnO_(2)纳米片的复合纳米材料。三金属Au@PdPt纳米颗粒提高了催化活性,花状MnO_(2)纳米片具有大的活性表面积能有效阻止Au@PdPt纳米颗粒聚集。因此,该纳米复合材料表现出较高的催化活性,增强的电子转移能力并有效地固定了抗体,从而放大了电流信号。基于上述优点,制备的免疫传感器表现出从1 pg·mL^(-1)到100 ng·mL^(-1)的宽浓度范围和0.76 pg·mL^(-1)的低检测限。此外,这种无标记免疫传感器具有高灵敏度、良好的选择性和长期稳定性,在生物测定分析中具有广阔的应用前景。

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

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.

Catalytic performance enhancement by alloying Pd with Pt on ordered mesoporous manganese oxide for methane combustion

Ordered mesoporous Mn2O3 (meso‐Mn2O3) and meso‐Mn2O3‐supported Pd, Pt, and Pd‐Pt alloy x(PdyPt)/meso‐Mn2O3; x = (0.10?1.50) wt%; Pd/Pt molar ratio (y) = 4.9?5.1 nanocatalysts were prepared using KIT‐6‐templated and poly(vinyl alcohol)‐protected reduction methods, respectively.The meso‐Mn2O3 had a high surface area, i.e., 106 m2/g, and a cubic crystal structure. Noble‐metalnanoparticles (NPs) of size 2.1?2.8 nm were uniformly dispersed on the meso‐Mn2O3 surfaces. AlloyingPd with Pt enhanced the catalytic activity in methane combustion; 1.41(Pd5.1Pt)/meso‐Mn2O3gave the best performance; T10%, T50%, and T90% (the temperatures required for achieving methaneconversions of 10%, 50%, and 90%) were 265, 345, and 425 °C, respectively, at a space velocity of20000 mL/(g?h). The effects of SO2, CO2, H2O, and NO on methane combustion over1.41(Pd5.1Pt)/meso‐Mn2O3 were also examined. We conclude that the good catalytic performance of1.41(Pd5.1Pt)/meso‐Mn2O3 is associated with its high‐quality porous structure, high adsorbed oxygen species concentration, good low‐temperature reducibility, and strong interactions between Pd‐Pt alloy NPs and the meso‐Mn2O3 support.

The Synthesis of Sub-Nano-Thick Pd Nanobelt-Based Materials for Enhanced Hydrogen Evolution Reaction Activity

Tailoring atomic structures of noblemetal nanomaterials with size close to single-unit cell range is essential in both fundamental researchand applications,including their development into high catalytic performance materials in renewable,green energy conversions,devices for energy storage,and as biosensors for environmental pollutants.However,several strategies used in fabricating these materials still impose enormous challenges,arising from lack of even size distribution,shape uniformity,and controlled composition,which are critical in determining their specific activities and efficiencies.Herein,we report a facile approach for preparing sub-nano-thick palladium nanobelt-based(PdNB)materials.Then we rationalized the formation mechanism of such highly anisotropic structures by morphology-related thermodynamic and kinetic analysis.Moreover,we investigated if electrocatalysis performance of these NB-basedmaterialswere enhanced.Thepalladium(Pd)NBs featured a thickness of∼0.9-1.2 nm and width of 5-18nmwith length extending to severalmicrometers[denoted as Pd(0.9)],or a thickness of∼0.7-0.9 nm and width of 2.5-6 nmwith length of several hundreds of nanometers[denoted as Pd(0.7)].According to our theoretical analysis,one-dimensional(1D)growth encountered almost no energy barrier at optimal reaction conditions,whereas the growth of Pd nanostructures with other dimensions confronted high barriers,indicating that it was plausible to prepare 1D structures with sizes close to single-unit cells.Also,platinum(Pt)could be successfully doped into the Pd(0.9)NBs through a galvanic epitaxial growth,forming edge-Pt-enriched Pd NBs(eePtPd NBs).Further,electron transfer from Pd to Pt imparted the eePtPd NBs with high hydrogen evolution reaction(HER)activity.The eePtPd NBs showed a 3.5 and 1.8 times higher in exchange current density and mass activity(at−0.1 V),respectively,compared to those of Pt catalysts in perchloric acid(HClO_(4))solutions.Finally,the NBs all showed high activity toward ethanol and formic acid oxidation reactions.Our current work aids in gaining insights into tailoring Pd nanostructures at an atomic level and provides Pd sub-nanometric 1D structures for further research.Moreover,our morphology-related thermodynamic and kinetic analysis extend our understanding of the control of nanostructure morphology and might shed light on the precision of designing specific morphologies of noble metal nanocrystal structures.