CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yongying Wang,Yangge Guo,Zhengwei Zhang,Zirui Wu,Chanez Maouche,Shuiyun Shen,Yi Li,Junliang Zhang,Juan Yang
Designing catalysts with high activity and stability to boost their ethanol oxidation reaction (EOR) performance is one of the central targets in the development of direct ethanol fuel cells (DEFCs). However, how to design the EOR catalysts in a rational way is still challenging, needing more efforts put in. Herein, we have synthesized a catalyst of PtCu-SnO 2 aerogel via ingeniously introducing Cu into Pt-SnO 2 system, resulting in the formation of a main phase of alloy (PtCu)-amorphous oxide (a-SnO 2 ) interface. Benefiting from the optimized structures, the PtCu-SnO 2 aerogel displays excellent acidic EOR performance with 4.5 times promotion in activity compared to pure Pt aerogel. In-depth investigations through electrochemical in-situ Fourier transform infrared spectroscopy and density functional theory calculations have shown that the absorbed OH on a-SnO 2 surface together with the greatly-modified electronic structure of the alloy surface atoms can facilitate the C1 pathway and the oxidation of *CO intermediates for ethanol oxidation reaction. The resulting affinity of surface OH and the modification of reaction energies both in turn contribute to the improvement of EOR performance with high activity, stability, and anti-poisoning ability, proving interfacial engineering an effective strategy for the rational design of EOR catalyst.
研究领域:
材料科学
·
电化学
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
FARADAY DISCUSSIONS
·
2021
·Vol. 233
·232-243
·
IF 4.008
Pengfei Yao,Jing Cao,Mingbo Ruan,Ping Song,Xue Gong,Ce Han,Weilin Xu
Achieving a highly efficient and durable methanol electro-oxidation catalyst in acid media is critical for the practical utilization of direct methanol fuel cells (DMFCs) at the commercial scale. Herein, we report a facile and effective one-pot strategy for the synthesis of carbon-supported PtCu alloy nanoparticles (PtCu NPs) with a Pt-rich surface, small particle size and uniform dispersion. The as-prepared PtCu NPs with the optimal alloy composition (Pt2Cu) exhibit a significantly improved electrochemical methanol oxidation reaction performance in terms of a high activity, superior CO tolerance and remarkable durability, in contrast to those of commercial Pt/C catalysts in acid media. Particularly, the Pt2Cu/C catalyst exerts a 4.5 times enhancement in the mass activity and a larger If/Ib value compared to those of commercial Pt/C (Pt/Ccomm). The enhanced catalytic activities can be ascribed to the high utilization of Pt and the high index facets of the surface. Also, the addition of Cu downshifts the d-band center of Pt and improves the CO tolerance during the methanol oxidation reaction process. This work provides an efficient strategy for designing desired Pt-based alloys for various catalytic reactions.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Small
·
2024
·
IF 13
Yangyang Ren,Beibei Li,Guichao Zhang,Zunming Lu,Lanlan Li,Xiaojing Yang,Xinghua Zhang,Xiaofei Yu
Improvement in the durable and active low-Pt nanocatalysts for oxygen reduction reaction (ORR) is the essential target for clean energy. Herein, an efficient CeO 2 supported PtCu alloy catalyst (PtCu/CeO 2 -C) for ORR in acid media is developed. The CeO 2 support can effectively anchor the PtCu particles and inhibit their migration during the long-life cycling, which is beneficial to the catalytic performance. According to the electrochemical experiments, the specific and mass activities of PtCu/CeO 2 -C are 1.09 mA cm −2 and 0.49 A mg Pt −1 at 0.9 V, which are 9.9 and 6.1 times as large as that of Pt/C, demonstrating its outstanding ORR activities in acid media. Moreover, the theoretical studies confirm that oxygen vacancies (V O ) as Lewis acid sites can facilitate the adsorption and dissociation of O 2 , regulate the electronic structure of Pt, and thus endow PtCu/CeO 2 -C with an efficient 4-electron ORR pathway. The results suggest that the rational design of supported Pt-based catalysts is of great significance for efficient ORR reaction.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Theranostics
·
2018
·
IF 8.537
Jinghua Li,Xiangyang Zu,Gaofeng Liang,KeKe Zhang,Yuliang Liu,Ke Li,Zhong Luo,Kaiyong Cai
Heavy atom nanoparticles have high X-ray absorption capacity and near infrared (NIR) photothermal conversion efficiency, which could be used as radio-sensitizers. We hypothesized that concave PtCu octopod nanoframes (OPCNs) would be an efficient nanoplatform for synergistic radio-photothermal tumor ablation. Methods: In this study, we newly exploited a folic acid-receptor (FR) mediated photothermal radiotherapy nanoagent base on OPCNs. OPCNs were synthesized with a hydrothermal method and then modified with polyethylene glycol (PEG) and folic acid (FA). A series of physical and chemical characterizations, cytotoxicity, targeting potential, endocytosis mechanism, biodistribution, systematic toxicological evaluation, pharmacokinetics, applications of OPCNs-PEG-FA for in vitro and in vivo infrared thermal imaging (ITI)/photoacoustic imaging (PAI) dual-modal imaging and synergistic photothermal radiotherapy against tumor were carried out. Results: The OPCNs-PEG-FA demonstrated good biocompatibility, strong NIR absorption and X-ray radio-sensitization, which enabling it to track and visualize tumor in vivo via ITI/PAI dual-modal imaging. Moreover, the as-synthesized OPCNs-PEG-FA exhibited remarkable photothermal therapy (PTT) and radiotherapy (RT) synergistic tumor inhibition when treated with NIR laser and X-ray. Conclusion: A novel multifunctional theranostic nanoplatform based on OPCNs was designed and developed for dual-modal image-guided synergistic tumor photothermal radiotherapy.
研究领域:
肿瘤学
·
生物医学工程
·
纳米医学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Xian Liu,Like Chen,Yang Yang,Liping Xu,Junyong Sun,Tian Gan
Rational tailoring of hollow and porous bimetallic structures with excellent electrocatalytic performance is appealing yet challenging. Further, combining independent bimetallic nanoparticles with flexible two-dimensional substrate by forming stable heterocomplex is still highly desired for electrocatalysis. Herein, hierarchical PtCu alloy octahedrons with hollow interiors and nanosheet-assembled nanoshells were synthesized by a facile and efficient chemical transformation strategy using Cu 2 O as sacrificial templates. Such octahedral PtCu nanocages displayed significantly enhanced electrocatalytic activity owing to their unique hollow and porous architectures which provided easy access for analytes to the catalyst surface. Thereafter, introduction of Ti 3 C 2 T x MXene was realized via simple incubation of Ti 3 C 2 T x in solution containing the 3-aminopropyltriethoxysilane-capped PtCu, and their electrostatic interaction guaranteed the firm adsorption of PtCu nanocages on Ti 3 C 2 T x nanosheets. It turned out that the sensitivity of the hybrid sensor was remarkably improved for electrochemical monitoring of endocrine disrupting pollutants in water, exhibiting ultrawide linear ranges and sub-nanomole detection limits. The eminent electrode performance is attributed to the high specific area, fast electrochemical kinetics, decent electrical catalytic ability, and the synergistic effect between Pt, Cu, and MXene.
研究领域:
材料科学
·
环境科学
·
分析化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Nano Materials
·
2024
·
IF 5.3
Congyue Sun,Zhongcheng Zhao,Dongyan Xu,Xiaojin Li,Ke Ye
The rapid development of proton-exchange membrane fuel cells needs to develop Pt-based oxygen reduction reaction (ORR) catalysts with activity and stability. In this study, PtCu alloy nanoparticles were in situ anchored on an N-doped porous carbon (NC) derived from ZIF-8 with a chemical reduction method to produce a PtCu/NC catalyst with a Pt loading of 7.96 wt %. The PtCu alloy nanoparticles are uniformly immobilized on the NC with a high surface area via a metal–support interaction. The electrochemical test results demonstrated that the PtCu/NC catalyst displays remarkable activity with an E1/2 value of 0.913 V vs RHE, higher than 0.878 V vs RHE for the commercial Pt/C. The ORR mass activity of the PtCu/NC catalyst is 1.49 and 6.54 times that of PtCu/XC-72 and commercial Pt/C, respectively. The eminent ORR performance of PtCu/NC is attributed to the high specific area of NC and electron-rich Pt sites enhanced by electron transfer from the N and Cu atoms. Moreover, PtCu/NC exhibited better catalytic stability than PtCu/XC-72 and Pt/C after 3000 potential cycles, attributed to the interaction between the N atom and PtCu alloy.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Kai An,Hongyan Jia,Ruobing Cheng,Yong Guo,Xiaohui Liu,Yanqin Wang
Pt-based bimetallic catalysts have gained more and more attention in propane dehydrogenation (PDH), but still suffer from the high cost and poor stability. In this work, a PtCu@S-1 catalyst with an extremely low loading of Pt (0.047 wt%) is prepared by in-situ hydrothermal synthesis and employed in PDH. An excellent productivity (propylene yield: 471.8 molC 3 H 8 ⋅ g Pt -1 ⋅ h −1 ) is achieved at 600 °C with a weight hour space velocity of 25.80 h −1 . After 50 h of reaction at 600 ℃, 0.047Pt0.19Cu@S-1 catalyst still remains sinter-free, with a deactivation rate of only 0.006 h −1 . Various characterizations show that Cu 0 co-existed with Pt 0 in PtCu@S-1 catalyst plays an important role, greatly improved catalyst reactivity and stability. At high weight hour space velocity (44.5 h −1 ), the propylene productivity can reach 1056.4 molC 3 H 8 ⋅ g Pt -1 ⋅ h −1 . This work provides a new way for the design of extremely low Pt-loaded PDH catalysts with excellent performance at high temperatures.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2021
·
IF 7.46
Huiyi Yang,Qiyi He,Junkang Pan,Mingxia Lin,Zhiting Lao,Qinglan Li,Xiping Cui,Suqing Zhao
Nanozymes are a type of artificial enzymes that can replace traditional natural enzymes for biotechnology to biosensing, biocatalysis , and biological imaging. Nevertheless, it is still a huge challenge in the pursuit of new mimic enzymes or multiple enzyme-like activities mimics. In this work, PtCu nanocages (PtCu NCs) with hollow interior and rough exterior was prepared. PtCu NCs displayed superior tetra-enzyme mimetic activities including peroxidase (POD)-, superoxide dismutase (SOD)-, catalase (CAT)- and ascorbic acid oxidase (AAO)-like activities. Meaningfully, attributed to the POD mimic activity, sensitive and convenient colorimetric biosensors for L -Cysteine ( L -Cys), homocysteine (Hcy) and glutathione (GSH) were developed with wide linear range (LR) and low limit of detection (LOD) of 0.28 μM, 1.48 μM and 0.75 μM (S/N = 3), respectively. Moreover, based on the AAO mimic activity, the cascade reaction was proposed including the oxidation of ascorbic acid (AA) to dehydroascorbic acid (DHAA) by PtCu NCs and the formation of the fluorescent quinoxaline (DFQ) coming from the reaction between DHAA and o-phenylenediamine (OPD). A novel fluorescent biosensor for dehydroepiandrosterone (DHEA) was successfully constructed based on the immunoassay method combined with the cascade reaction for AA, with the LR of 0.6–464.9 ng·mL −1 and LOD of 0.5 ng·mL −1 . These colorimetric and fluorescent biosensors displayed outstanding performance in terms of sensitivity, specificity, and accuracy for real samples, suggesting that PtCu NCs was a promising candidate for biosensing.
研究领域:
生物传感
·
纳米材料
·
医学检测
✓ 已验证
产品关联
DOI
高影响因子
Nanoscale Advances
·
2020
·Vol. 2
·期 4
·1603-1612
·
IF 0
Haiyan Xiang,Yueshao Zheng,Yue Sun,Tingting Guo,Pei Zhang,Wei Li,Shiwei Kong,Miray Ouzounian,Hong Chen,Huimin Li,Travis Shihao Hu,Gang Yu,Yexin Feng,Song Liu
Designing effective catalysts by controlling morphology and structure is key to improving the energy efficiency of fuel cells. A good understanding of the effects of specific structures on electrocatalytic activity, selectivity, and stability is needed. Here, we propose a facile method to synthesize PtCu bimetallic nanostructures with controllable compositions by using Cu nanowires as a template and ascorbic acid as a reductant. A further annealing process provided the alloy PtCu with tunable crystal structures. The combination of distinct structures with tunable compositions in the form of PtCu nanowires provides plenty of information for better understanding the reaction mechanism during catalysis. HClO4 cyclic voltammetry (CV) tests confirmed that various phase transformations occurred in bimetallic and alloy samples, affecting morphology and unit cell structures. Under a bifunctional synergistic effect and the influence of the insertion of a second metal, the two series of structures show superior performance toward methanol electrooxidation. Typically, the post-product alloy A-Pt14Cu86 with a cubic structure (a = 3.702 Å) has better methanol oxidation reaction (MOR) catalysis performance. Density functional theory (DFT) calculations were performed to determine an optimal pathway using the Gibbs free energy and to verify the dependence of the electrocatalytic performance on the lattice structure via overpotential changes. Bimetallic PtCu has high CO tolerance, maintaining high stability. This work provides an approach for the systematic design of novel catalysts and the exploration of electrocatalytic mechanisms for fuel cells and other related applications.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
JOURNAL OF ALLOYS AND COMPOUNDS
·
2021
·
IF 5.316
Jinghua Li,Jianbo Zhang,Xibin Jiao,Jiahua Shi,Jiangxue Ye,Kena Song,Jianfeng Bao,Guangda Li,Kun Lei
In this work, near-infrared (NIR) light driven concave octopod PtCu alloy nanocages (OPtCu-NCs) were fabricated and first developed as photothermal synergetic Fenton catalyst for degradation of pollutant dyes. Moreover, by irradiating with NIR laser (808 nm), the obtained OPtCu-NCs exhibit excellent NIR absorption capacity and thus produce hyperpyrexia over 50 °C. Concomitantly, by the photothermal effect, the OPtCu-NCs nanocatalysts was used for elimination of organic dyes such as Methylene blue (MB) and Rhodamine B (RhB). The NIR-driven photothermal degradation mechanism under NIR irradiation can be attributed to the Fenton-like catalytic performance of Cu ions , then -N C- and/or C-C bonds in the molecular skeleton were fractured and electrons were donated intensively. As confirmed by a typical radical trapping experiment, electrons trigger the formation of miscellaneous reactive species (O 2 - , HO 2 , especially •OH) subsequently . Moreover, the photothermal Fenton-catalytic activity of the as-prepared OPtCu-NCs had maintained at 93.15% (for MB) and 91.87% (for RhB) after ten circulating degradation processes. All acquired results reveal that the OPtCu-NCs have the potential applied value in dyestuff-wastewater treatment under neutral pH.
研究领域:
环境科学
·
纳米材料
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Nano
·
2023
·
IF 17.1
Mingze Sun,Shuyan Gong,Zhengwen Li,Helai Huang,Yanjun Chen,Zhiqiang Niu
The activity and stability of the platinum electrode toward the oxygen reduction reaction are size-dependent. Although small nanoparticles have high Pt utilization, the undercoordinated Pt sites on their surface are assumed to have too strong oxygen binding strength, thus often leading to compromised activity and surface instability. Herein, we report an extended nanostructured PtCu ultrathin surface to reduce the number of low-coordination sites without sacrificing the electrochemical active surface area (ECSA). The surface shows (111)-oriented characteristics, as proven by electrochemical probe reactions and spectroscopies. The PtCu surface brings over an order of magnitude increase in specific activity relative to commercial Pt/C and nearly 4-fold enhancement in ECSA compared to traditional thin films. Moreover, due to the weak absorption of air impurities (e.g., SO2, NO, CO) on highly coordinated sites, the catalyst displays enhanced contaminant tolerance compared with nanoparticulate Pt/C. This work promises a broad screening of extended nanostructured surface catalysts for electrochemical conversions.
研究领域:
材料科学
·
电化学
·
催化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Rongxiu Guo,Xinyue Zhang,Ze-Nan Hu,Hong Li,Jianyi Gao,Jiaping Wang,Qionglin Liang,Xiaodong Li,Dun Niu,Hong-bin Sun
Hollow metal nanoparticles have attracted great interest in heterogeneous catalysis research due to their unique structures as nanoreactors. Here, we report hollow PtCu nanoparticles encapsulated in microporous silica shells (H-PtCu@SiO 2 ), which can serve as the nanoreactor with high catalytic activity and high stability. The H-PtCu@SiO 2 nanoreactor shows the state-of-the-art catalytic performance for the transfer hydrogenation of benzonitrile to dibenzylamine, which achieves up to 100% conversion and 99% selectivity in only 0.5 h. The void-confinement effect of H-PtCu@SiO 2 is crucial for the outstanding catalytic performance by encaging the reactants in the nanoreactor. The computation demonstrates the limiting diffusion effect of the silica shell toward the ammonia borane, thus reduces the concentration of reductant species and prolongs the lifetime of the intermediate imine to improve the selectivity of secondary amine. Moreover, the silica shells can effectively enhance the catalytic stability of the H-PtCu@SiO 2 nanoreactor.
研究领域:
化学工程
·
催化材料
·
纳米技术
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）