Nanoscale Advances
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2022
·Vol. 4
·期 16
·3362-3369
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IF 5.598
Dancheng Zhu,Kai Zheng,Jun Qiao,Hao Xu,Chao Chen,Pengfei Zhang,Chao Shen
Owing to their enhanced catalytic stability and cyclability, two-dimensional (2D) material-supported Pd-based bimetallic alloys have promising applications for catalytic reactions. Furthermore, the alloying strategy can effectively reduce costs and improve catalytic performance. In this paper, we report a one-step reduction method to synthesize a novel heterogeneous catalyst, PdCu@Ti3C2, with good catalytic performance. The composition and structure of the as-prepared catalyst were characterized by inductively coupled plasma-mass spectrometry (ICP-MS), scanning transmission electron microscopy (STEM), energy-dispersive X-ray spectroscopy (EDX), and X-ray photoelectron spectroscopy (XPS). The catalyst particles, which were identified as a PdCu bimetallic alloy, exhibited good dispersion on the substrate. The performance of the catalyst in the Suzuki–Miyaura coupling reaction was studied, and the results showed that PdCu@Ti3C2 had excellent catalytic activity, similar to that of homogeneous Pd catalysts such as Pd(PPh3)4. Moreover, the prepared catalyst could be reused at least 10 times in the Suzuki–Miyaura coupling reaction with high yield.
研究领域:
化学
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材料科学
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PubMed
高影响因子
ELECTROCHIMICA ACTA
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2020
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IF 6.215
Na Ye,Zhao Jiang,Tao Fang
Direct methanol fuel cells (DMFCs) have attracted extensive attention due to clean, efficient characteristics and portable applications. In this work, a series of Pd x Cu y /reduced graphene oxide (rGO) catalysts are assembled and the catalytic performances are investigated for methanol oxidation reaction (MOR) in alkaline media. The intrinsic surface electronic structures of the Pd x Cu y /rGO bimetallic catalysts are also studied to clarify the reaction mechanism. The results reveal that Pd 1.2 Cu 0.2 /rGO exhibits superior catalytic activity (1101.58 A g Pd −1 ), 4.2 and 5.2 times higher than those of the commercial PtRu/C and Pd/C catalysts. CO stripping suggests that the onset potential for CO oxidation on the Pd 1.2 Cu 0.2 /rGO catalyst is lower than those on the commercial PtRu/C and Pd/C catalysts, implying that the anti-CO poisoning ability is enhanced. Combined with the analysis of X-ray diffraction (XRD), high-resolution transmission electron microscopy (HRTEM), X-ray photoelectron spectroscopy (XPS) and Raman, the enhanced catalytic activity and anti-CO poisoning ability are attributed to the charge transfer and lattice compression between Pd and Cu, which modify the d-band center and weaken the adsorption of CO. Furthermore, a volcano plot is found between the MOR activity and d-band center, indicating that the excellent MOR activity is attributed to the optimal d-band center with the moderate adsorption strength of CO-like intermediates.
研究领域:
材料科学
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电化学
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催化反应
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DOI
高影响因子
ELECTROCHIMICA ACTA
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2020
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IF 6.215
Shaoda Huang,Shuanglong Lu,Hongyin Hu,Binbin Cao,Huining Li,Fang Duan,Han Zhu,Hongwei Gu,Mingliang Du
Palladium-based catalyst represents one of the most promising candidates among all non-platinum oxygen reduction reaction (ORR) catalysts. However, it is still challenging to precisely engineering their morphology and composition . Herein, highly branched core-shell PdCu@Pd nanocrystals have been fabricated via a simple one-pot synthesis that co-directed by hydrogen gas and halide ions. Such unique PdCu@Pd nanocrystals exhibit prominent ORR activity, durability and methanol-tolerance in alkaline media owing to their core-shell composition , highly-branched structure and defect-rich surface. This work elucidates a facile strategy to design highly branched core-shell nanomaterials , shedding light on the exploration and optimization of novel non-platinum ORR catalysts.
研究领域:
材料科学
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电化学
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催化科学
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DOI
高影响因子
ACS Applied Materials & Interfaces
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2020
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IF 8.758
Tianxing Yang,Yuliang Feng,Rui Ma,Qiang Li,Hong Yan,Yanan Liu,Yufei He,Jeffrey T. Miller,Dianqing Li
In this work, a simple post-treatment has been carried out on a solid palladium–copper alloy to enhance the ethylene selectivity without any loss of activity. In all catalysts, PdCu/C catalysts post-treated at 375 °C exhibit improved ethylene selectivity (86%) compared to the solid PdCu/C catalysts (61%) at 100% acetylene conversion with comparable catalytic activity. During the post-treatment, the average size of PdCu nanoparticles is maintained at 6.6–6.8 nm, and no obvious segregation is observed. X-ray photoelectron spectroscopy and in situ extended X-ray absorption fine structure (EXAFS) results display that Pd is in a metallic state for all PdCu catalysts before and after post-treatment. Moreover, the EXAFS fitting results show that the Pd–Pd bond is gradually replaced by the Pd–Cu bond. The good separation of Pd atoms by Cu is also proven by XRD characterization, which shows that a body-centered cubic PdCu structure with uniform distribution of Pd and Cu in a unit cell forms under 375 °C post-treatment. The rearrangement of Pd and Cu atoms has a limited impact on the surface Pd dispersion, avoiding the activity loss due to the decrease in Pd sites. The improved selectivity could be attributed to the isolation of Pd and the accompanied d-band center downshifting, which favors the desorption of π-bonded ethylene species.
研究领域:
催化化学
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材料科学
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高影响因子
APPLIED SURFACE SCIENCE
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2019
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IF 5.155
Dengfeng Wu,Daojian Cheng
Herein, we introduce a facile strategy for the structure-controlled synthesis of one-dimensional PdCu nanocrystals via a seed-mediated approach. This developed strategy involves the synthesis of Cu nanowires with penta-twinned structure, and subsequent growth of Pd metal on Cu nanowires. The obtained one-dimensional PdCu nanocrystals are of rough surfaces and core-shell like architecture. Upon the tuning reactivity of (111) and (100) crystal faces on Cu nanowires in absence or presence of capping agent, one-dimensional PdCu nanocrystals with solid or hollow interiors (nanowires or nanotubes) can be controllably synthesized through galvanic displacement reaction, respectively. It is found that both PdCu nanowires and PdCu nanotubes exhibit better performance for oxygen reduction reaction compared with self-synthesized PdCu nanoparticles and commercial Pd/C in 0.1 M KOH electrolyte. Particularly, PdCu nanotubes show Pt-like performance, and achieve an onset potential of 0.941 V ( vs. RHE) and a half potential of 0.825 V. The electron transfer number during oxygen reduction is close to 4 on PdCu nanotubes. Moreover, the catalytic stability of the obtained one-dimensional PdCu nanocrystals is much superior to that of commercial Pd/C and Pt/C catalysts.
研究领域:
材料科学
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化学
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高影响因子
INORGANIC CHEMISTRY
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2025
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IF 4.7
Changjin Xu,Yinglei Liu,Huiqing Guo,Chun Du,Gaowu Qin,Song Li
The ability to finely tune the nuclearity of active metal sites is critical for designing highly selective catalysts, especially for hydrogenation processes. In this work, we developed a novel PdCu catalyst with an ordered body-centered cubic (BCC) structure, enabling precise control over Pd nuclearity to optimize selectivity. Using a facile polyol synthesis method, we modulated the Pd coordination environment, reducing the Pd–Pd coordination number from 3 (disordered face-centered cubic, FCC) to 0 (ordered BCC), thereby achieving full isolation of Pd by the surrounding Cu atoms. This structural transformation enhances hydrogen spillover and weakens ethylene adsorption, resulting in superior activity for the selective hydrogenation of acetylene to ethylene. The ordered PdCu supported on Al2O3 (o-PdCu/Al2O3) achieved a 99% acetylene conversion with an 84.5% ethylene selectivity at near-room temperature. This work highlights the importance of controlling atomic-scale nuclearity in metal catalysts and provides a promising strategy for improving the catalytic efficiency and selectivity in industrially significant processes.
研究领域:
催化化学
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材料科学
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PubMed
高影响因子
ACS Catalysis
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2026
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IF 13.6
Fan Chen,Jinming Wang,Yuan He,Dandan Liu,Lin Hu,Rui Shi,Yana Liu,Jiguang Zhang,Yunfeng Zhu,Jun Wang
Photocatalytic aerobic oxidation of methane (CH4) to methanol (CH3OH) offers an alternative to the current energy-intensive route for CH4 utilization, while suffering from the activity-selectivity trade-off due to the uncontrolled generation of reactive oxygen species (ROS). Herein, we perform the photocatalytic CH4 aerobic oxidation in the presence of H2 over a PdCu NPs-modified ZnO catalyst, which exhibits a CH3OH yield of 13.5 mmol gcat–1 h–1 and a selectivity of 71.1%, surpassing many previously reported results. The introduction of H2 enables more ROS production simultaneously from photoelectron-induced O2 reduction and in situ-produced H2O2, facilitating the conversion of CH4. Compared to Pd, the PdCu cocatalyst favors the generation of more •OOH radicals in the ROS. More importantly, it is proposed that intermediate CH3OOH can be converted to CH3OH by H2-derived Pd–H species, which could also scavenge the excessive •OH radicals and holes, thus promoting the productivity of CH3OH and suppressing overoxidation. This work provides a strategy to regulate ROS formation for efficient CH4 oxidation into CH3OH under mild conditions.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2026
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IF 12.5
Haoye Wang,Bowen Yang,Yanxi Qi,Richard L. Smith,Yaqiong Su,Xinhua Qi
Self-supported PdCu-based multi-component alloys bifunctional electrodes were fabricated by electrodeposition. • A paired electrochemical system realized upcycling of waste PET plastic and nitrate-containing wastewater. • The high-entropy effect regulated the electronic structure of PdCu alloys and enhanced the catalytic activity. With the continuous decrease in the cost of renewable electricity, the electrocatalytic coupling systems provide a sustainable strategy for treating Poly(ethylene terephthalate) (PET) waste plastic and nitrate-polluted wastewater. However, their practical application depends on bifunctional electrocatalysts with high selectivity and stability. Herein, a self-supported high-entropy-like PdCu-based multi-component alloy (PdCuFeCoNi) electrode is fabricated via a one-step electrodeposition, achieving Faradaic efficiencies of 92.1% for NH 3 and 96.8% for GA production. The incorporation of Fe, Co, and Ni induces a high-entropy-like effect that regulates the electronic structure of the PdCu-based multi-component alloy, downshifts the d-band center, enhances the adsorption of *EG and *OH, and promotes the conversion of the key intermediate *CO-CH 2 OH to GA. For nitrate reduction reaction (NO 3 RR), a cooperative tandem mechanism between Cu sites facilitating the adsorption of NO 3 − and Pd promoting water dissociation enables the conversion of NO 3 − → NO 2 − → NH 3 . In the flow-coupled two-electrode reactor using PdCuFeCoNi alloy electrode as both cathode and anode, the NO 3 RR//EGOR system requires a cell voltage of only 0.52 V to achieve 100 mA cm −2 , which is 1.09 V lower than that of traditional NO 3 RR system, indicating that this coupled system can simultaneously carry out the upgrading pathways of waste plastics and nitrate wastewater with economic viability. The high-entropy-like effect regulates the electronic structure of PdCu alloy electrodes, enhancing the reaction kinetics of multi-component PdCu-based alloys in the electrochemical upcycling of PET plastic waste and nitrate wastewater. Download: Download high-res image (153KB) Download: Download full-size image
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Shuqian Xie,Jinbing Shu,Hui Huang,Junhong Li,Ruirui Yue,Jingkun Xu
Improving the electrocatalytic performance by modulating the surface and interface electronic structure of noble metals is still a research hotspot in electrocatalysis . Herein, we prepared the heterogeneous catalyst based on the well-dispersed PdCu nanoalloy and the N -doped Ti 3 C 2 T x MXene support (PdCu/N-Ti 3 C 2 T x ) via in situ growth of PdCu nanoparticles on the fantastic N-Ti 3 C 2 T x sheets. By exploring the electrocatalytic properties of ethanol oxidation reaction (EOR), the composition optimized Pd 1 Cu 1 /N-Ti 3 C 2 T x delivers higher mass activity/specific activity/intrinsic activity (2200.7 mA mg Pd -1 /13.1 mA cm −2 /2.2 s −1 ), anti-poisoning ability and stability than those of Pd/N-Ti 3 C 2 T x , Pd 1 Cu 1 /Ti 3 C 2 T x and commercial Pd/C, which can be attributed to the modified surface electronic features of Pd by the participation of Cu atoms and N-Ti 3 C 2 T x MXene , as well as the “metal-carrier” effect between the PdCu nanoalloy and N-Ti 3 C 2 T x heterogeneous interface. Furthermore, the conductivity of N-Ti 3 C 2 T x MXene can be improved by N -doping, and the abundant terminal groups (-O, –OH, -F and N) on the N-Ti 3 C 2 T x surface can promote the electron exchange between PdCu and N-Ti 3 C 2 T x . This work provides an effective strategy for engineering heterogeneous electrocatalysts for enhanced electrocatalytic EOR by adjusting the interfacial electronic structure of noble metals.
研究领域:
电催化
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材料科学
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化学工程
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高影响因子
ACS Applied Materials & Interfaces
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2024
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IF 8.3
Zheng Tang,Yongjia Li,Lanlan Shi,Kaixin Zhang,Yingjie Ji,Xiaoxuan Wang,Yebo Yao,Xia Liu,Dewei Wang,Kaiqi Nie,Jiangzhou Xie,Zhiyu Yang,Yi-Ming Yan
Direct formate fuel cells have gained traction due to their eco-friendly credentials and inherent safety. However, their potential is hampered by the kinetic challenges of the formate oxidation reaction (FOR) on Pd-based catalysts, chiefly due to the unfavorable adsorption of hydrogen species (Had). These species clog the active sites, hindering efficient catalysis. Here, we introduce a straightforward strategy to remedy this bottleneck by incorporating Pd with Cu to expedite the removal of Pd–Had in alkaline media. Notably, Cu plays a pivotal role in bolstering the concentration of hydroxyl adsorbates (OHad) on the surface of catalyst. These OHad species can react with Had, effectively unblocking the active sites for FOR. The as-synthesized catalyst of PdCu/C exhibits a superior FOR performance, boasting a remarkable mass activity of 3.62 A mg–1. Through CO-stripping voltammetry, we discern that the presence of Cu in Pd markedly speeds up the formation of adsorbed hydroxyl species (OHad) at diminished potentials. This, in turn, aids the oxidative removal of Pd–Had, leveraging a synergistic mechanism during FOR. Density functional theory computations further reveal intensified interactions between adsorbed oxygen species and intermediates, underscoring that the Cu–Pd interface exhibits greater oxyphilicity compared to pristine Pd. In this study, we present both experimental and theoretical corroborations, unequivocally highlighting that the integrated copper species markedly amplify the generation of OHad, ensuring efficient removal of Had. This work paves the way, shedding light on the strategic design of high-performing FOR catalysts.
研究领域:
催化
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电化学
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材料科学
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燃料电池
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理论化学
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PubMed
高影响因子
BIOSENSORS & BIOELECTRONICS
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2015
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IF 6.409
Yuanyuan Liu,Hongmin Ma,Jian Gao,Dan Wu,Xiang Ren,Tao Yan,Xuehui Pang,Qin Wei
In this study, a novel and ultrasensitive sandwich-type electrochemical immunosensor was designed for the quantitative detection of squamous cell carcinoma antigen (SCCA) based on the β-cyclodextrin functionalized graphene nanosheet (CD-GN) and the ternary hollow Pt/PdCu nanocube anchored on three-dimensional graphene framework (Pt/PdCu-3DGF). CD-GN exhibited high specific surface area and good dispersibility and stability in water, which were beneficial to fix captured antibodies (Ab 1 ) through the supramolecular host-guest interaction between CD and Ab 1 . The abundant oxygen-containing functional groups on 3DGF provided binding sites for anchoring noble metal nanoparticles . Pt/PdCu-3DGF could capture detected antibodies via the interaction of Pd-NH 2 and Pt-NH 2 . Furthermore, the ternary metal nanoparticles exhibited high electrocatalytic activity toward the reduction of hydrogen peroxide. Under optimal conditions, the fabricated immunosensor showed a sensitive response to SCCA with two linear ranges. The linear ranges are 0.0001–1 ng/mL and 1–30 ng/mL with a detection limit of 25 fg/mL. Additionally, the proposed immunosensor showed good reproducibility and stability.
研究领域:
生物化学
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医学检测
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纳米技术
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PubMed
高影响因子
危险品化学品经营许可证（带存储）