ACS Catalysis
·
2024
·
IF 11.3
Xiashuang Luo,Cehuang Fu,Shuiyun Shen,Xiaohui Yan,Liuxuan Luo,Junliang Zhang
A comprehensive understanding of the intricate surface environments of practical nanocatalysts at the atomic level is essential for advancing our knowledge of catalytic mechanisms. In this study, we investigate PtCu octahedral nanoparticles with varying microstrains engineered by Cu dispersion. A detailed analysis of the atom configuration and corresponding microstrain is conducted. The intimate mixing of Cu and Pt results in increased randomness in atom displacement within the lattice and a more pronounced distribution of alternating microstrain on the surfaces. Specifically, we observe that the PtCu concave octahedral nanoparticles with alternating microstrain demonstrate a substantial oxygen reduction reaction (ORR) activity of 3.95 mA cm–2 in area-specific activity. The significant impact of shear microstrain is further underscored, as evidenced by an 86.9% decrease in the ORR activity upon the removal of the alternating shear microstrain. This study sheds light on the effects of microstrain toward the ORR and provides valuable insights into designing advanced Pt-based electrocatalysts.
研究领域:
材料科学
·
电化学
·
催化科学
✓ 已验证
DOI
高影响因子
AUSTRALIAN JOURNAL OF CHEMISTRY
·
2018
·Vol. 71
·期 7
·504-510
·
IF 1.059
Yanna Hu,Taiyang Liu,Chaozhong Li,Qiang Yuan,Yanna Hu,Taiyang Liu,Chaozhong Li,Qiang Yuan
Sponge-like metal nanomaterials have been paid great attention due to their unique structure for wide applications in hydrogen storage, filtration, sensors, heterogeneous catalysis, and fuel cells. Here, we first use a facile, bottom-up method to successfully prepare composition-tunable PtCu alloy nanosponges constructed with sub-4.5 nm particle building blocks. Due to the porous structure, structure defects, and synergetic effect of Pt and Cu, the PtCu alloy nanosponges exhibit good electrocatalytic performances towards methanol oxidation. Compared with pure Pt nanosponges, the specific/mass activity on PtCu2 alloy nanosponges is 5.84/2.93 times that on pure Pt nanosponges. Furthermore, the stability and reactivation ability of PtCu alloy nanosponges are also superior to pure Pt nanosponges.
研究领域:
材料科学
·
燃料电池技术
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Hongyu Wang,Kai Zhang,Lanlan Wu,Yanji Wang,Xiaohang Du,Jingde Li
The development of active and durable low-Pt electrocatalysts for oxygen reduction reaction (ORR) is the key target for proton exchange membrane fuel cells. Herein, a charge transfer and spillover effect enabled efficient ordered porous titanium dioxide supported PtCu alloy-based carbon-free ORR catalyst (PtCu@TiO 2-x N) is developed. Experimental characterization and theoretical analysis reveal that the rich oxygen vacancies and N-doping of TiO 2 support promotes the electron transfer from PtCu to TiO 2-x N, resulting in electron-deficient PtCu surface. This weakens the adsorption of ORR intermediates on PtCu, and simultaneously promotes their spillover from PtCu sites to adjacent TiO 2-x N support. This dynamic renewal of the PtCu active sites allows the rapid proceed of ORR, and thus accelerating its reaction kinetics. Accordingly, the PtCu@TiO 2-x N catalyst exhibits greatly enhanced ORR activity with a specific activity of 1.83 mA cm −2 Pt , mass activity of 1.24 A mg −1 Pt and excellent durability as well. The results show that the rational design of Pt-based catalyst with spillover effect is of great significance towards efficient ORR reaction.
研究领域:
材料科学
·
电化学
·
催化作用
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
XiaShuang Luo,CeHuang Fu,ShuiYun Shen,LiuXuan Luo,JunLiang Zhang
Hollow metal–based nanoparticles usually possess improved electrocatalytic properties, but challenge in their tedious and complicated synthetic protocols. In this paper, a one–step template–free method is newly developed, whereby the N–doped PtCuCo polycrystalline nanospheres can be spontaneously transformed to the N–doped PtCuCo porous hollow nanospheres . Specifically, the Kirkendall voids form with the rapid removal of transition metals in the starting nanoparticles by a special diffusion–oxidation–complexation effect. The N–doped Pt 7 Cu hollow nanospheres with ultrathin porous shells are formed after removing the surface oxides. A large electrochemical surface area of 97.9 m 2 g Pt –1 is established with the formation of abundant open channels in the hollow nanospheres. With the synergetic effect of the introduction of Cu, N components and the high Pt utilization, the N–doped Pt 7 Cu porous hollow nanospheres demonstrate greatly enhanced electrocatalytic mass activities of 2.14 A mg Pt –1 and 1.42 A mg Pt –1 toward ethanol oxidation and oxygen reduction reactions, respectively.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
RSC Advances
·
2021
·Vol. 11
·期 42
·26326-26335
·
IF 3.361
Yongxiao Tuo,Qing Lu,Chen Chen,Tenglong Liu,Yuan Pan,Yan Zhou,Jun Zhang
Pt is the most efficient electrocatalyst for the hydrogen evolution reaction (HER); however, it is a high cost material with scarce resources. In order to balance performance and cost in a Pt-based electrocatalyst, we prepared a series of PtCu bimetallic nanoparticles (NPs) with different Pt/Cu ratios through a facile synthetic strategy to optimize the utilization of Pt atoms. PtCu NPs demonstrate a uniform particle size distribution with exposed (111) facets that are highly active for the HER. A synergetic effect between Pt and Cu leads to electron transfer from Pt to Cu, which is favorable for the desorption of H intermediates. Therefore, the as-synthesized carbon black (CB) supported PtCu catalysts showed enhanced catalytic performance in the HER compared with a commercial Pt/C electrocatalyst. Typically, Pt1Cu3/CB showed excellent HER performance, with only 10 mV (acid) and 17 mV (alkaline) overpotentials required to achieve a current density of 10 mA cm−2. This is because the Pt1Cu3 NPs, with a small average particle size (7.70 ± 0.04 nm) and Pt–Cu core and Pt-rich shell structure, display the highest electrochemically active surface area (24.7 m2 gPt−1) out of the as-synthesized PtCu/CB samples. Furthermore, Pt1Cu3/CB showed good electrocatalytic stability, with current density drops of only 9.3% and 12.8% in acidic solution after 24 h and in alkaline solution after 9 h, respectively. This study may shed new light on the rational design of active and durable hydrogen evolution catalysts with low amounts of Pt.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
PubMed
高影响因子
Advanced Materials Interfaces
·
2021
·Vol. 8
·期 11
·2100013
·
IF 6.147
Rongxiu Guo,Guangqi He,Xinyu Chen,Xinyue Zhang,Ze-nan Hu,Xiaodong Li,Dun Niu,Hong-bin Sun
Surface wettability of heterogeneous catalysts plays a crucial role in the catalytic activity and selectivity. In this work, an ultra-thin modified silica coating is firstly used as the “skin” to adjust the surface hydrophilicity of the catalyst, which promotes the catalytic activity and selectivity in the transfer hydrogenation of nitriles. The ultrathin-modified silica “skin” with 2–3 nm thickness is fabricated by the consecutive hydrolysis of (3-aminopropyl)triethoxysilane and n -propyltriethoxysilane, and the bimetallic catalyst Fe 3 O 4 @PtCu is encapsulated in the coating. The modified catalyst demonstrated significant catalytic efficiency for hydrogenation of benzonitrile to dibenzylamine. The reaction performs 93% conversion and 99% selectivity in “green” solvent H 2 O. Furthermore, the modified silica “skin” encapsulates the PtCu nanoparticles to prevent the leaching of active sites, thus brings excellent catalytic recyclability. More than Fe 3 O 4 @PtCu, the modified silica “skin” is applicable to a diverse range of catalysts, that is, PtCu/SiO 2 , PtCu/Al 2 O 3 , and PtCu/UiO-66, endowing them with additional catalytic activity and selectivity in the hydrogenation of nitriles.
研究领域:
催化
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2019
·Vol. 9
·期 61
·35887-35894
·
IF 3.049
Ting Bian,Biao Sun,Sai Luo,Long Huang,Shan Su,Chunfeng Meng,Shichuan Su,Aihua Yuan,Hui Zhang
Pt-based nanocrystals with a twinned structure are highly desirable to achieve high performances in both catalytic activity and durability for methanol oxidation reaction (MOR). However, it still remains great challenge for producing such twinned nanocrystals due to the high internal strain energy of Pt. Here we present a seed-mediated approach to generate Au@PtCu nanostars with a five-fold twinned structure using Au decahedra as seeds. The composition of Pt/Cu in the nanocrystals was tuned by varying the molar ratio of Pt to Cu salt precursors with the amount of Au seeds being the same. Through composition optimization, Au@Pt1.2Cu nanostars achieved the highest specific (1.06 mA cm−2) and mass (0.18 mA mgPt−1) activities for MOR, which were about 5.9 and 1.6 times higher than those of commercial Pt/C, respectively. After accelerated stability test (ADT) for 1500 cycles, such nanostars remained ∼95% of specific activity compared to a loss of ∼28% for commercial Pt/C, indicting their superior durability for MOR. We believed that this enhancement may arise from the unique twinned structure and possible synergetic effect between Pt and Cu components.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Xue Li,Jingjia Zhang,Qianhui Li,Shuimei Yang,Chengze Wei,Feng Zhang,Zhenbo Wang
Preparing low-cost and high-activity methanol oxidation reaction (MOR) electrocatalysts is a key approach for renewable energy technologies. However, due to the high price and instability of platinum-based catalysts, the addition of transition metals to alloy catalysts on the basis of platinum is a prevalent strategy to improve catalytic activity and stability. Herein, we prepared a PtCu alloy catalyst that is highly dispersed on an N-doped carbon dodecahedron (PtCu/N-DC) by a simple pyrolysis method. The experiments demonstrate that the robust interaction between N-doped porous carbon support and PtCu alloy imparts strong stability to the catalyst. At the same time, there is a strong interaction between Cu atom and Pt atom, doping with Cu can adjust its surface electronic configuration of Pt, thereby improving the MOR performance of the catalyst. With a platinum loading of just 10 % compared to the 20 % in commercial Pt/C, PtCu/N-DC exhibits mass activity and specific activity that are 4.1 times and 5.8 times higher, with significant catalytic activity and a high level of resistance to carbon monoxide poisoning. Theoretical analysis indicates that the PtCu/N-DC catalyst exhibits a low energy barrier during the critical steps, which aligns with the enhanced electrocatalytic activity demonstrated in the experimental findings.
研究领域:
材料科学
·
电化学
·
可再生能源技术
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Qingrong Long,Chaoyang Shi,Dawei Zhang,Danyang Wei,Haoqi Li,Linxiang Zhou,Hanyu Tan,Jie Yu,Mingli Xu
The frequently used chloroplatinic acid or other Pt precursors containing Cl element during the preparation process of Pt-based catalysts lead to catalyst poisoning and instability. In this work, a chlorine-free PtCu(N)/C R-F catalyst with a hollow sphere structure was successfully synthesized by employing [Pt(NH 3 ) 4 ](OH) 2 and [Cu(NH 3 ) 4 ](OH) 2 as the chlorine-free metal precursors, which using the strong electrostatic adsorption (SEA) between positively charged metal precursor ions and the negatively charged oxygen-containing functional groups (OCFGs) on the carbon support (C R-F ) and combined with the impregnation reduction method. Compared to commercial Pt/C, the experimental results show that the PtCu(N)/C R-F catalyst, displays better ORR performance under acidic condition, the onset and half-wave potentials are 0.961 V (vs. RHE) and 0.827 V (vs. RHE), respectively. Furthermore, it also shows a significant performance advantage in a gas diffusion electrode (GDE) half-cell. Density-functional theory (DFT) calculations show that the introduction of Cu has adjusted the electronic structure of Pt, weakened the adsorption of oxygen-containing intermediates, and ultimately enhanced the catalytic activity and stability of ORR. This work presents a simple and efficient method for preparing chlorine-free Pt-based catalysts.
研究领域:
材料科学
·
催化化学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
ANALYTICA CHIMICA ACTA
·
2023
·
IF 6.2
Shida Cao,Hongli Zhao,Kaicha Chen,Fangfang Zhou,Minbo Lan
Adenosine, as an endogenous nucleoside modulator , plays an important role in heart rate regulation, neurotransmission , and control of the respiratory system and thus it is significantly important to realize its sensitive detection . Herein, a highly sensitive electrochemical aptasensor for adenosine detection was proposed by using multi-walled carbon nanotubes (MWCNTs) as support matrix loading PtCu nanoparticles (PtCu-MWCNTs) to amplify signal. On one hand, disposable screen-printing gold electrodes (SPGEs) were used as superb sensing base to ensure the stable connection of aptamers 1 (ssDNA1). On the other hand, the PtCu-MWCNTs complex was synthesized through a one-pot method, which not only can precisely control the proportion of metal mass in the product but also exhibited superior electrocatalytic activity towards H 2 O 2 . The recognition reactions were achieved by stepwise incubation of ssDNA1, ssDNA2-PtCu-MWCNTs (denoted as ssDNA2-label), and adenosine on the SPGEs. As a result, the constructed electrochemical aptasensor exhibited a wide linear range from 10 nM to 1.0 μM with a low detection limit of 1.0 nM (S/N = 3) for adenosine detection. The aptasensor also successfully realized the adenosine detection in human serum samples, which means that the proposed aptasensor holds a potential application in point-of-care detection.
研究领域:
生物化学
·
医学诊断
·
纳米技术
·
电化学分析
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nanoscale
·
2023
·Vol. 15
·期 36
·14931-14940
·
IF 6.7
Xiang Long,Yang Yang,Zhen-Long Dou,Qu-Quan Wang,Li Zhou
Heterocrystals consisting of multiple species have received wide attention owing to the advantage of the cooperative effect contributed by different functional counterparts; therefore, a controlled growth strategy is highly desired. Herein, we report an effective method to synthesize dumbbell-like Au–PtCu solid and hollow nanorods, regulated by the unique surface capping and oxidation etching roles of copper ions. Dumbbell-like nanorods are prepared through site-selective co-deposition of platinum and copper on both tips of gold nanorods assisted by the capping effect of the CTAB–Cu+ complex to passivate the side surface. On the other hand, hollow dumbbell-like Au–PtCu nanorods are formed through triggering the etching effect of copper ions by increasing the reaction temperature to 80 °C. The manipulation of the morphology and extinction properties of the trimetallic Au–PtCu nanorods is demonstrated by adjusting the concentration of copper ions. Under excitation with a near-infrared 808 nm laser, the dumbbell-like Au–PtCu nanorods show excellent photothermal conversion, with a 3.1 times temperature increment (ΔT) compared to bare Au nanorods, while the hollow dumbbell-like Au–PtCu NRs demonstrate improved photocatalytic activity under xenon lamp irradiation.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2015
·
IF 7.435
Zhi Liang Zhao,Lian Ying Zhang,Shu Juan Bao,Chang Ming Li
Metal core–shell nanostructures have been extensively studied as one of the most promising electrocatalysts to significantly reduce the loading of the expensive Pt catalyst for fuel cells but it is very challenging to fabricate such a structure to possess proper metal components while making small and uniformly distributed nanoparticles for high catalytic performance. In this work, small and uniformly distributed Au-core/PtCu alloy–shell structured nanoparticles (Au@PtCu NPs) were fabricated by a novel one-pot facile method. The as-prepared Au@PtCu/C has a much larger electrochemical active surface area (ECSA) (64.8 m 2 g −1 Pt ) than that of AuPtCu/C(38.5 m 2 g −1 Pt ), PtCu/C (31.02 m 2 g −1 Pt ) and commercial Pt/C (25.4 m 2 g −1 Pt ) catalyst. This new catalyst not only greatly reduces Pt loading but also significantly increases the catalytic activity and stability toward methanol oxidation reaction in comparison to the commercial electrocatalyst. This is mainly attributed to a synergistic effect from the small and uniform core–shell nanostructure and the unique chemical compositions of Au and PtCu alloy, thus offering a great potential for a less expensive but highly active catalyst toward direct methanol fuel cells (DMFCs).
研究领域:
材料科学
·
能源科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）