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Materials · 2025 ·Vol. 18 ·期 6 ·1279 · IF 3.2

One-Pot Synthesis of Pd@Pt Core-Shell Icosahedron for Efficient Oxygen Reduction

Zisheng Tang,Dafu Zhao,Xiaoqian Wang,Yanhui Jiao,Manrui Liu,Chengqi Liu,Qi Zhang,Shujing Ren,Yong Liu

Enhancing the limited utilization and overall yield of Pt-based catalysts is essential for advancing proton exchange membrane fuel cell technology. Herein, we report a facile one-pot method that utilizes TEG as both a solvent and a reductant to efficiently synthesize a Pd@Pt core-shell icosahedron. By controlling the surface energy between Pd and Pt precursors, we achieved the formation of Pd@Pt core-shell icosahedra, resulting in a fourfold reduction in reaction time and an eightfold increase in yield. Moreover, the core-shell structures exhibited a significant enhancement in electrocatalytic activity, stability, and Pt utilization efficiency. In comparison to commercial Pt/C, the Pd@Pt core-shell icosahedron exhibited efficient mass activity (MA, 1.54 A mg−1Pt) and specific activity (SA, 2.24 mA cm−2Pt) at 0.9 V (vs. RHE), while demonstrating excellent stability with minimal loss of activity even after 10,000 potential cycles. The Pd@Pt icosahedra configuration integrates the advantages of multiply twinned nanostructures, leading to rich electrochemical active surface sites and fast charge transport, thereby improving its catalytic performance and long-term stability during electrocatalytic reactions.

研究领域: 材料科学 · 能源化学 · 电催化
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BIOSENSORS & BIOELECTRONICS · 2013 · IF 5.437

“Turn off–on” fluorescent sensor for platinum drugs-DNA interactions based on quantum dots

Dan Zhao,Jiaotian Li,Tianming Yang,Zhike He

A “turn off–on” mode has been established by using the interaction between platinum anticancer drugs and DNA as input signal and the fluorescence reversible change of quantum dots (QDs) as output signal. The QDs fluorescence can be quenched by platinum anticancer drugs via photo-induced electron transfer process, rendering the system into “turn off” status, and the system can then be “turned on” when fluorescence is restored due to covalent conjugation between DNA and platinum anticancer drugs. This dual-directional fluorescence change realized the detection of cisplatin and DNA, overcoming the selectivity problem commonly existed in the traditional mono-directional fluorescence detection mode. The reversible fluorescent “turn off-on” mode has been further employed to study the interactions between DNA and different platinum anticancer drugs (cisplatin, oxaliplatin and carboplatin). Furthermore, the impacts of different types of DNAs (different in base sequence , chain length and ssDNA/dsDNA) on the mode are also explored. This simple, fast and convenient spectroscopic method owns promising applications in the study on interaction between medical molecules and DNA, and in biochemical detections.

CAS / MDL: 127-09-3
研究领域: 化学 · 生物化学 · 药学 · 分子生物学
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ELECTROCHIMICA ACTA · 2023 · IF 6.6

The underlying mechanism trade-off between particle proximity effect and low-Pt loading for oxygen reduction and methanol oxidation reaction activity

Jiarun Cheng,Chaojie Lyu,Gang Dong,Yongqiang Liu,Yue Hu,Bin Han,Dongsheng Geng,Dongjie Zhao

Highly efficient and stable Pt-based electrocatalysts have broad application prospects in fuel cells, among which, Pt loading accompanied with particle size, interparticle distance (ipd), and interaction with support are identified as key contributors for high activity and selectivity. Herein, we have developed the nitrogen-doped graphite-like carbon sheets supporting low-Pt loading (Pt@N-GC) with uniform size and controllable ipd, and disentangled the main effect of ipd on oxygen reduction reaction (ORR) and methanol oxidation reaction (MOR) activity. The optimal 5.0 wt% low-Pt loading results in more abundant Pt sites and lower ipd, which leads to the higher surface reactivity by proximity effect , and 2e − pathway can be hindered by strongly resorbing and reducing H 2 O 2 to promote 4e − pathway towards ORR . Simultaneously, the 5.0 wt% Pt@N-GC can effectively improve the MOR activity, enhance the adsorption of -OH group under the appropriate ipd, so as to promote the instantaneous oxidation of CO and enhance the tolerance, and accelerate the oxidative dehydrogenation of methanol. Benefiting by the synergistic effect of Pt nanoparticles and N-GC support, all Pt@N-GCs exhibit bifunctional electrocatalytic activity and durability. We believe the gained trade-off of the loading and proximity effect of Pt, and its influence on catalytic activity and selectivity contributes to design more promising low-Pt loading bifunctional catalysts for fuel cell.

研究领域: 材料科学 · 电化学
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ACS Applied Energy Materials · 2025 · IF 5.5

Preparation of High-Platinum-Load Platinum-on-Carbon Catalysts by Liquid-Phase Pressurized Hydrogen Reduction Using Platinum Nitrate Impregnation and High Specific Surface Area Carbon Carriers

Yongmi Wang,Shihao Fan,Bing Fan,Weifeng Liu,Lin Chen,Duchao Zhang

High Pt-load catalysts can be used to prepare thin catalytic layers and high-energy-density proton-exchange-membrane fuel cell cathodes for practical applications. However, because high Pt loads agglomerate Pt nanoparticles on carrier surfaces, the batch preparation of high Pt-load catalysts possessing both high activity and high Pt nanoparticle dispersibility is important for practical applications. In this study, high Pt-load Pt/C catalysts were prepared using a platinum nitrate precursor and the high specific surface area Ketjenblack EC600JD carbon carrier via impregnation and liquid-phase hydrogenation reduction. In the catalyst, the average Pt nanoparticle size was 2.30 nm. The electrochemically active surface area of the Pt/CEC600JD catalyst was 63.91 m2 gPt–1, and its mass activity (MA) was 0.35 A mgPt–1 at 0.9 V (versus a reversible hydrogen electrode), which is 1.4 times that of commercial 50% Pt/CTKK, as measured using a rotating disk electrode. After 20 000 accelerated durability test cycles, the MA of the Pt/CEC600JD catalyst was 1.7 times that of 50% Pt/CTKK under the same experimental conditions. The catalyst synthesized using platinum nitrate and EC600JD showed excellent activity and can be used for practical electrocatalytic applications.

CAS / MDL: 16941-12-1 18496-40-7
研究领域: 材料科学 · 电化学
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Catalysts · 2024 ·Vol. 14 ·期 6 ·344 · IF 3.8

Ionic Liquid Modification of High-Pt-Loading Pt/C Electrocatalysts for Proton Exchange Membrane Fuel Cell Application

Fengshun Cheng,Yuchen Guo,Xinhong Liang,Fanqiushi Yue,Yichang Yan,Yang Li,Yuanzhi Zhu,Yanping He,Shangfeng Du

Ionic liquid modification for carbon-supported platinum (Pt/C) electrocatalysts to enhance their oxygen reduction reaction (ORR) activity has been well recognized. However, the research has only been reported on the low-Pt-loading Pt/C electrocatalysts, e.g., 20 wt%, while in practical applications, usually high-Pt-loading Pt/C electrocatalysts of 45–60 wt% are used. In this work, ionic liquid modification is systematically investigated for a Pt/C electrocatalyst with 60 wt% Pt loading for its ORR activity in the cathode in proton exchange membrane fuel cells (PEMFCs). Various adsorption amounts are studied on the catalyst surface. Different modification behavior is found. Mechanism exploration shows that the adsorption of ionic liquid mainly happens on the Pt electrocatalyst surface and in the micropores of the carbon support. The highest fuel cell power performance is achieved at an ionic liquid loading of 7 wt%, which is much higher than the 3 wt% reported for the low-Pt-loading Pt/C.

CAS / MDL: 31175-20-9
研究领域: 能源科学 · 材料科学 · 化学工程
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International Journal of Electrochemical Science · 2023 · IF 1.5

One-step Hydrothermal Synthesis of Ultralow Pt Loading Ni(OH)2 for Enhanced Hydrogen Evolution Reaction

Jiao Chen,Hongye Qin,Yaping Pan,Jinli Wu,Jianan Liu,Wanying Lin,Jun Jiang,Enzuo Liu,Junwei Sha,Fang He,Liying Ma,Naiqin Zhao

It is necessary and challenging to develop platinum-based electrocatalysts with low Pt content and high performance for industrial development in a suitable strategy. Herein, ultralow Pt (0.35 wt%) loading Ni(OH) 2 nanosheets (named as 2-Pt/Ni(OH) 2 ) with cataphracted structure is synthesized on nickel foam by one-step hydrothermal process. It only needs an overpotential of 34 mV to achieve a current density of 10 mA cm -2 without any significant decrease for 40 hours. This excellent performance of hydrogen evolution reaction (HER) is attributed to the fact that the cataphracted structure not only has a larger active area and more active sites, but also effectively limits the size of Pt nanoparticles to 2~3 nm, which results in a higher active quality. In addition, the relatively simple and easily operational one-step method can reduce the Pt content to 0.35 wt% significantly. This facile strategy opens up new approaches in the rational design and synthesis of low loading Pt electrocatalysts with eminent electrocatalytic activity for industrial production.

研究领域: 材料科学 · 电化学
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NEW JOURNAL OF CHEMISTRY · 2020 ·Vol. 44 ·期 15 ·5792-5799 · IF 3.288

A facile solvothermal synthesis of Pt1.2Co/C bimetallic nanocrystals as efficient electrocatalysts for methanol oxidation and hydrogen evolution reaction

Xilong Wang,Chen Yang,Lijuan Cao,Han-Pu Liang

Alloying Pt with less expensive 3d-transition metals is effective for increasing the electrocatalytic activity and CO tolerance while decreasing Pt consumption. Herein, well-dispersed and highly alloyed Pt–Co bimetallic nanoparticles supported on commercial carbon black have been synthesized by means of a facile one-pot solvothermal approach without using any bulky capping agents. The best performing Pt1.2Co/C, with an average particle size of 4.7 ± 0.8 nm, has a large electrochemically active surface area of 64.30 m2 g−1, which is comparable to that of 66.73 m2 g−1 of commercial Pt/C and larger than that of other synthesized catalysts. The as-synthesized Pt1.2Co/C shows about 3 times enhanced mass activity and specific activity for methanol oxidation reaction compared to commercial Pt/C (20 wt%). Meanwhile, the electrocatalytic performance of Pt1.2Co/C for hydrogen evolution reaction (HER) in acid media is also superior to commercial Pt/C and the overpotential is only 33.8 mV when the current density reaches 70 mA cm−2. This work demonstrates that the developed strategy provides a facile platform for the synthesis of high-performance, low-cost and robust catalysts in practical catalysis, and energy storage and conversion.

CAS / MDL: 65-85-0 68-12-2
研究领域: 材料科学 · 电化学 · 能源转换与存储
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ACS Catalysis · 2015 · IF 9.312

Kinetically Stabilized Pd@Pt Core–Shell Octahedral Nanoparticles with Thin Pt Layers for Enhanced Catalytic Hydrogenation Performance

Peipei Zhang,Yibo Hu,Baihai Li,Qiuju Zhang,Chen Zhou,Hongbo Yu,Xuejun Zhang,Liang Chen,Bryan Eichhorn,Shenghu Zhou

This study investigates the structural stability of small Pd@Pt core@shell octahedral nanoparticles (NPs) and their shell thickness dependent catalytic performance for p-chloronitrobenzene hydrogenation with H2. The 6–8 nm Pd@Pt octahedral NPs are prepared by a sequential reduction method, and the characterization results confirm that Pd@Pt octahedral NPs with one to four atomic Pt layers can be controllably synthesized. The Pd@Pt octahedral NPs with one atomic Pt layer demonstrate excellent structural stability with the maintenance of core–shell structures as well as high catalytic stability during cycle to cycle catalytic p-chloronitrobenzene hydrogenation reactions. The alumina-supported Pd@Pt octahedral NPs illustrate a superior catalytic performance relative to individual Pt and Pd and their physical mixtures. Theoretical calculations by density functional theory suggest that the unexpected structural stability for Pd@Pt octahedral NPs with thin Pt shells and their corresponding catalytic stability during hydrogenation reactions can be ascribed to the strong binding between Pt surfaces and reactants/products in catalytic reactions. The enhanced catalytic performance of Pd@Pt octahedral NPs possibly originates from the core–shell interaction, which adjusts the electronic state of surface Pt atoms to be suitable for selective p-chloronitrobenzene hydrogenation.

CAS / MDL: 7647-10-1 16919-58-7
研究领域: 材料科学 · 催化化学 · 理论计算
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2021 · IF 8.128

Engineering intermetallic-metal oxide interface with low platinum loading for efficient methanol electrooxidation

Wei Zhao,Li Ma,Mengyu Gan,Xudong Li,Yuchao Zhang,Xuelian Hua,Ling Wang

Constructing a distinctive electrochemical interface with low platinum content to boost the sluggish methanol electrooxidation kinetics is critical for commercializing the direct methanol fuel cells. Herein, we have synthesized highly active electrocatalysts with unique intermetallic-metal oxide interfaces through a facile pyrolysis method. Physical characterizations demonstrate that the obtained PtFe (1:2) @a-FeO x /NC-C catalyst with low platinum content of 7.2 wt% possesses an interfacial structure composed of face-centered tetragonal ( L 1 0 ) PtFe intermetallic nanoparticles accompanied with amorphous iron oxide . Electrochemical measurements show that the synthesized PtFe (1:2) @a-FeO x /NC-C catalyst not only exhibits excellent methanol electrooxidation activities with a mass activity of 1.48 A mg -1 Pt and a specific activity of 2.34 mA cm -2 Pt in acid medium, but also possesses better CO-tolerant performance and faster methanol oxidation kinetics compared with commercial Pt/C. The improved electrochemical performances may ascribe to the modified electronic structure by alloying platinum with iron and the special PtFe@a-FeO x interface, which render strong synergistic interactions between bimetallic PtFe nanoparticles and amorphous iron oxide. Consequently, the presented strategy offers new prospects into the construction of low-cost electrocatalysts with unique electrochemical interface for enhancing catalytic performances.

CAS / MDL: 461-58-5
研究领域: 材料科学 · 电化学
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APPLIED ORGANOMETALLIC CHEMISTRY · 2020 ·Vol. 34 ·期 8 ·e5680 · IF 3.14

Synthesis, characterization, and biological activity of new mixed ammine/amine platinum(IV) complexes

Chunyan Jia,Yanwei Cong,Shaoping Pu,Linxiang Cai,Yunshuang Zhong,Xinzhong Zhang,Xiali Liao,Yamin Li,Bo Yang,Chuanzhu Gao

A series of mixed ammine/amine platinum(IV) complexes with lipophilic ligands in their axial positions were designed, synthesized, and spectrally characterized. In vitro cytotoxicity evaluation of these complexes and their lead compounds have been carried out against A549, SMMC-7721, MCF-7, and SW480 human cancer cell lines. The introduction of carboxylate ions as leaving group can improve the aqueous solubility and stability of the platinum(II) complexes. The carboxylato ligands and chloride ligands in the axial position markedly increased the lipophilicity and cytotoxicity of compounds C4 and C5. Particularly, compound C5 showed two to eight times higher cytotoxicity than cisplatin and satraplatin against selected cell lines. For its oral activity and no cross-resistance potentiality, C5 is expected to be an antitumor platinum drug candidate. This novel class of platinum compounds represents a valuable lead in the development of new-generation agents capable of demonstrating cytotoxicity superior to that of the clinically established cisplatin.

研究领域: 化学 · 药学 · 肿瘤学
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Nature Communications · 2022 ·Vol. 13 ·期 1 ·1-16 · IF 17.694

A nuclease-mimetic platinum nanozyme induces concurrent DNA platination and oxidative cleavage to overcome cancer drug resistance

Li Fangyuan,Sun Heng,Ren Jiafeng,Zhang Bo,Hu Xi,Fang Chunyan,Lee Jiyoung,Gu Hongzhou,Ling Daishun

Platinum (Pt) resistance in cancer almost inevitably occurs during clinical Pt-based chemotherapy. The spontaneous nucleotide-excision repair of cancer cells is a representative process that leads to Pt resistance, which involves the local DNA bending to facilitate the recruitment of nucleotide-excision repair proteins and subsequent elimination of Pt-DNA adducts. By exploiting the structural vulnerability of this process, we herein report a nuclease-mimetic Pt nanozyme that can target cancer cell nuclei and induce concurrent DNA platination and oxidative cleavage to overcome Pt drug resistance. We show that the Pt nanozyme, unlike cisplatin and conventional Pt nanoparticles, specifically induces the nanozyme-catalyzed cleavage of the formed Pt-DNA adducts by generating in situ reactive oxygen species, which impairs the damage recognition factors-induced DNA bending prerequisite for nucleotide-excision repair. The recruitment of downstream effectors of nucleotide-excision repair to DNA lesion sites, including xeroderma pigmentosum groups A and F, is disrupted by the Pt nanozyme in cisplatin-resistant cancer cells, allowing excessive accumulation of the Pt-DNA adducts for highly efficient cancer therapy. Our study highlights the potential benefits of applying enzymatic activities to the use of the Pt nanomedicines, providing a paradigm shift in DNA damaging chemotherapy.

研究领域: 癌症研究 · 纳米技术 · 药学 · 分子生物学
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Journal of the American Chemical Society · 2023 · IF 15

Platinum–Lead–Bismuth/Platinum–Bismuth Core/Shell Nanoplate Achieves Complete Dehydrogenation Pathway for Direct Formic Acid Oxidation Catalysis

Xinrui Hu,Zhengyi Xiao,Weizhen Wang,Lingzheng Bu,Zhengchao An,Shangheng Liu,Chih-Wen Pao,Changhong Zhan,Zhiwei Hu,Zhiqing Yang,Yucheng Wang,Xiaoqing Huang

Designing platinum (Pt)-based formic acid oxidation reaction (FAOR) catalysts with high performance and high selectivity of direct dehydrogenation pathway for direct formic acid fuel cell (DFAFC) is desirable yet challenging. Herein, we report a new class of surface-uneven PtPbBi/PtBi core/shell nanoplates (PtPbBi/PtBi NPs) as the highly active and selective FAOR catalysts, even in the complicated membrane electrode assembly (MEA) medium. They can achieve unprecedented specific and mass activities of 25.1 mA cm–2 and 7.4 A mgPt–1 for FAOR, 156 and 62 times higher than those of commercial Pt/C, respectively, which is the highest for a FAOR catalyst by far. Simultaneously, they show highly weak adsorption of CO and high dehydrogenation pathway selectivity in the FAOR test. More importantly, the PtPbBi/PtBi NPs can reach the power density of 161.5 mW cm–2, along with a stable discharge performance (45.8% decay of power density at 0.4 V for 10 h), demonstrating great potential in a single DFAFC device. The in situ Fourier transform infrared spectroscopy (FTIR) and X-ray absorption spectroscopy (XAS) results collectively reveal a local electron interaction between PtPbBi and PtBi. In addition, the high-tolerance PtBi shell can effectively inhibit the production/adsorption of CO, resulting in the complete presence of the dehydrogenation pathway for FAOR. This work demonstrates an efficient Pt-based FAOR catalyst with 100% direct reaction selectivity, which is of great significance for driving the commercialization of DFAFC.

研究领域: 材料科学 · 能源化学 · 催化科学
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