ACS Materials Au
·
2022
·
IF 0
Qingsong Luo,Hai Wang,Liang Wang,Feng-Shou Xiao
Selective hydrogenation of acetylene to ethylene is an industrially important process to purify the raw ethylene stream for producing high-grade polyethylene. The supported Pd catalyst exhibits superior activity for acetylene hydrogenation but suffers from poor ethylene selectivity because of the easy overhydrogenation to produce ethane. Here, we report that the PdCu alloy nanoparticles within siliceous zeolite crystals effectively tuned Pd-catalyzed overhydrogenation into semihydrogenation. This catalyst displayed an ethylene selectivity of 92.9% with a full conversion of acetylene. Mechanism studies reveal that the zeolite fixation stabilized the alloyed structure, where the electron-enriched Pd surface benefits the rapid ethylene desorption to hinder the deep hydrogenation. This work provides an efficient strategy for a rational design of bimetallic metal catalysts for selective hydrogenations.
研究领域:
催化化学
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材料科学
·
纳米技术
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DOI
NEW JOURNAL OF CHEMISTRY
·
2025
·
IF 2.5
Chenghu Zhang,Zezhou Xing,Ying Li,Tong Xu,Yinghui Sun,Jie Bai
Utilizing metal alloying strategies to fully exploit the role of precious metals in upgrading biomass chemicals remains both a challenging task and a key sustainable strategy. To improve the hydrogen transfer efficiency of furfural molecules in the catalytic transfer hydrogenation pathway, we report a Pd–Cu alloy composite nanocatalyst supported on mesoporous-structured zirconia through electrospinning technology. The chemical states of Pd and Cu in the catalyst were studied using XRD, HRTEM and XPS characterization methods, proving the presence of the PdCu alloy. A series of synthesized monometallic and bimetallic catalysts were tested for their ability to catalyze the catalytic transfer hydrogenation of furfural. Results showed that the PdCu alloy catalyst exhibited excellent performance similar to that of the monometallic Pd catalyst. 95.6% furfural conversion and 91.5% furfuryl alcohol selectivity were achieved at 170 °C and 2 MPa N2 for 12 h, and the catalytic activity did not decrease significantly after 6 cycles. The excellent catalytic activity was mainly attributed to the alloy and solvent effects, which promoted the improvement in hydrogen transfer efficiency.
研究领域:
化学工程
·
催化材料
·
生物质转化
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产品关联
DOI
高影响因子
Materials Chemistry Frontiers
·
2022
·Vol. 6
·期 16
·2190-2200
·
IF 8.683
Chengguang Liu,Xiaolei Guo,Zhen-Feng Huang,Jinheng Li,Li Gan,Lun Pan,Chengxiang Shi,Xiangwen Zhang,Guidong Yang,Ji-Jun Zou
Due to the utilization of renewable energy and proton sources, the electrochemical nitrogen reduction reaction is considered as an efficient, sustainable, and carbon-neutral route to replace the industrial Haber–Bosch process. However, restricted by the highly competitive hydrogen evolution reaction and the highly inert NN bond, electrochemical nitrogen reduction research still faces significant challenges with a low level of selectivity and activity. Herein, we demonstrate a catalyst (PdCu/TiO2−x) composed of oxygen vacancy-rich TiO2−x nanosheets and PdCu alloy nanoparticles by the co-reduction method of metal precursors. Such a catalyst exhibits excellent electrocatalytic performance at room temperature and pressure, with an NH3 yield rate of 8.51 mmol gcat−1 h−1 and the corresponding faradaic efficiency of 49.09% at −0.1 V vs. the reversible hydrogen electrode, which are much higher than most reported palladium-based catalysts and their alloy catalysts. Characterization and experimental results confirm that by properly constructing the surface defect and nanoalloy structure, the optimized electronic structure and synergistic effect can not only effectively improve the N2 adsorption and activation, but also reduce the reaction barrier, resulting in efficient electrocatalytic performance. Meanwhile, the introduction of Cu accelerates the hydrogen desorption, further effectively improving the faradaic efficiency. Overall, we explored the electrocatalytic performance and mechanism of the bimetal alloy catalyst, as well as the optimization strategies for enhancing the nitrogen mass transfer process, providing new insight into the rational design of a highly efficient e-NRR system through tuning of the catalyst and reaction environment.
研究领域:
材料科学
·
电化学
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产品关联
DOI
高影响因子
Nanoscale Advances
·
2022
·Vol. 4
·期 16
·3362-3369
·
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
·
材料科学
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产品关联
DOI
PubMed
高影响因子
ACS Applied Energy Materials
·
2018
·
IF 0
Shao-Qing Liu,Yi-Tao Xu,Jin-Qi Xie,Guo-Qing Sheng,Yan-Wu Zhu,Xian-Zhu Fu,Rong Sun,Ching-Ping Wong
Novel bowl-like, apple-like, and spherical PdCu alloy hollow microparticles with mesoporous nanoshells are synthesized through a simple disproportionation reaction route using a spherical Cu2O template with increasing H2PdCl4 ratio. The diameter of hollow particles is about 1 μm, and the thickness of mesoporous shells is about 50 nm. The obtained bowl-like PdCu alloy hollow microparticles with mesoporous nanoshells exhibit the highest electrocatalytic activity among the apple-like and spherical PdCu hollow microparticles and commercial Pd/C electrocatalysts toward methanol anodic oxidation for fuel cells. The remarkably excellent electrocatalytic performance of bowl-like PdCu alloy electrocatalysts might be attributed to the unique bowl-like hollow architecture with highly mesoporous nanoshells which are constructed by self-supported PdCu nanoparticles. The strategy presented here might help pave the way for the synthesis of novel nano-/microcomplex hollow materials with mesoporous nanoshells.
研究领域:
材料科学
·
电化学
·
纳米技术
✓ 已验证
DOI
ACS Applied Nano Materials
·
2024
·
IF 5.3
Xi Quan,Fa Guo,Ruru Li,Hao Zhang,Zhurui Shen,Jun Zhang
Optimization regarding the electronic structure of nanometal cocatalysts via alloying is considered as a promising strategy to regulate the formation of reactive oxygen species (ROS) in photocatalytic degradation. Herein, a series of g-C3N4-supported PdCu alloy cocatalysts were constructed to investigate the regulatory effect and mechanism of alloying on photocatalytic active species. Photocatalytic degradation experiments using ciprofloxacin (CIP) as a model pollutant demonstrated that optimal alloying with PdCu (Cu ≤ 0.5 wt %) significantly boosts the production of active species and incrementally enhances the contribution of superoxide anions (·O2–). The introduction of Cu leads to the redistribution of surface electrons in the PdCu alloy, resulting in a gradual strengthening of the O2 adsorption as the Cu content increases up to 0.5 wt %. The CIP degradation rate reaches a maximum of 80.5% at pH 6.7. Inorganic ions such as Na+ and Ca2+ inhibit degradation, while low concentrations of Fe3+ promote that. The CIP degradation rate in actual water samples ranges from 71.1 to 78.2%. Furthermore, the degradation pathway initiated from carbonyl destruction induced by a higher ·O2– concentration was proposed. This comprehensive study provides valuable insights into the design of alloyed photocatalysts, emphasizing the significance of optimizing metal composition to regulate ROS generation and enhance photocatalytic efficiency.
研究领域:
材料科学
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环境科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
·
2019
·Vol. 33
·期 11
·e5198
·
IF 3.259
Yu Ru,Yanli Huang,Yuanyuan Wang,Liyi Dai
Well distributed Pd-Cu bimetallic alloy nanoparticles supported on amine-terminated ionic liquid functional three-dimensional graphene (3D IL-rGO/Pd-Cu) as an efficient catalyst for Suzuki cross-coupling reaction has been prepared via a facile synthetic method. The introduction of IL-NH 2 cations on the surface of graphene sheets can effectively avoid the re-deposition of graphene sheets, allowing the catalyst to be reused up to 10 cycles. The addition of Cu not only saves cost but also ensures high catalytic efficiency. It is worthy to note that the catalyst 3D IL-rGO/Pd 2.5 Cu 2.5 can efficiently catalyze the Suzuki cross-coupling reaction with the yield up to 100% in 0.25 h, almost one-fold higher than that by the pristine IL-rGO/Pd 2.5 catalyst (52%). The Powder X-Ray Diffraction (XRD), combining energy dispersive X-ray spectroscopy (EDS) mapping results confirm the existence and distribution of Pd and Cu in the bimetallic nanoparticles. The transmission electron microscopy (TEM) reveals the nanoparticle size with an average diameter of 3.0 ± 0.5 nm. X-ray photoelectron spectroscopy (XPS) analysis proved the presence of electron transfer from Cu to Pd upon alloying. Such alloying-induced electronic modification of Pd-Cu alloy and 3D ionic liquid functional graphene with large specific surface area both accounted for the catalytic enhancement.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
·
IF 9.7
Shang-Xiong Wei,Yu-Hang Yang,Xue-Bo Liu,Xiao-Bin Ye,Xiao-Peng Zhao,Xue-Wei Pi,Xue-Feng Cheng,Jing-Hui He
The electrochemical reduction reaction of nitrate (NO 3 RR) to ammonia is an environmentally friendly approach that can treat wastewater as well as find an alternative to the energy-intensive Haber-Bosch process. The use of adhesives partially to adhere to the NO 3 RR electrocatalysts, leading to sluggish kinetics, poor stability and poor scalability. Herein, we report the synthesis of PdCu alloy catalysts via a direct laser writing method, demonstrating their exceptional performance in the electrochemical reduction of nitrate. The Pd 0.55 Cu 0.45 alloy exhibited a remarkable ammonia production rate of 30.55 mg h −1 cm −2 under neutral electrolyte conditions and maintained stable operation for over 1500 h. Density functional theory (DFT) calculations and experimental analyses revealed that the PdCu alloy’s enhanced activity stems from its lower energy barrier for the rate-determining step (*NO → *NOH) and improved mass transfer capabilities. The alloy’s electronic properties and geometric configuration, fine-tuned by the laser-induced synthesis method, facilitate the conversion of NO 2 − and suppress the hydrogen evolution reaction (HER), thereby significantly enhancing the selectivity and activity of the NO 3 RR process. This study provides a sustainable and efficient pathway for ammonia synthesis and offers insights into the design of advanced catalysts for environmental and energy applications.
研究领域:
环境科学
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电催化
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材料科学
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产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2016
·
IF 7.145
Shu-He Han,Juan Bai,Hui-Min Liu,Jing-Hui Zeng,Jia-Xing Jiang,Yu Chen,Jong-Min Lee
Noble metal nanostructures (NMNSs) play a crucial role in many heterogeneous catalytic reactions. Hollow and porous NMNSs possess generally prominent advantages over their solid counterparts due to their unordinary structural features. In this work, we describe a facial one-pot synthesis of hollow and porous Pd–Cu alloy nanospheres (Pd–Cu HPANSs) through a polyethylenimine (PEI)-assisted oxidation–dissolution mechanism. The strong coordination interaction between CuII and PEI facilitates the oxidation–dissolution of the Cu2O nanospheres template under air conditions, which is responsible for the generation of the Pd–Cu alloy and the convenient removal of the Cu2O nanospheres template at room temperature. Compared to the commercial Pd black, the Pd–Cu HPANSs show remarkably improved catalytic activity for the reduction of K2Cr2O7 by HCOOH at room temperature, attributing to the enhanced catalytic activity of the Pd–Cu HPANSs for the dehydrogenation decomposition of HCOOH.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Materials Today Sustainability
·
2022
·
IF 7.244
X. Tai,B. Wu,J. Bao,W. Qu,L. Zhao,Z. Wang
Rational synthesis of bimetallic electrocatalysts with the special geometric structure for direct formic acid fuel cells remains yet challenging. Herein, a facile synthetic strategy is presented to prepare the bimetallic Pd–Cu alloy nanospheres (Pd–Cu ANSs) catalysts based on the galvanic replacement and high-temperature reconstruction. The formation mechanism of Pd–Cu ANSs is studied thoroughly from comprehensive characterizations and control experiments. The optimized Pd–Cu ANSs with unique nanosphere structure as well as regulated electronic structure provide excellent electrocatalytic performance for formic acid oxidation reaction (FAOR) with a specific activity of 6.11 mA cm - 2 Pd and mass activity of 1569.48 mA mg -1 Pd , which are 2.7 times and 3.5 times as high as these of the Pd/C catalyst. This synthetic method outlined here could provide a new pathway for noble metal-based alloy nanomaterials for diverse applications.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Wenxia Fan,Ani Wang,Lei Wang,Xin Jiang,Zhenzhen Xue,Jinhua Li,Guoming Wang
Delicate design and bottom-up synthesis of hollow nanostructures for oxygen evolution electrocatalysts is a promising way to accelerate the reaction kinetics of overall water splitting. Herein, an efficient and versatile strategy for the controllable preparation of Pd–Cu alloy nanoparticles encapsulated in carbon nanopillar arrays (PD–Cu@HPCN) is developed. Core–shell structured MOF@imidazolium-based ionic polymers (ImIPs) have been prepared and adopted as a template, along with the decomposition of the inner Cu–MOFs when an anion exchange occurs between sodium tetrachloropalladate in solution and bromides in the external ImIP shell. Pd nanoparticles will be highly dispersed in the resulting Pd–Cu@HO-ImIP array, and subsequent topotactic transformation generates Pd–Cu@HNPC. No hazardous reagents or tedious steps are used to remove the inner Cu–MOF templates in contrast to the traditional top-down methods. Remarkably, the Pd–Cu@HPCN catalyst possesses outstanding oxygen evolution reaction (OER) activity, including small overpotential with 10 mA cm–2 at an overpotential of 188 mV, a large double layer capacitance (73.8 mF cm–2), and high stability (20 h). This simple, green, and efficient synthesis methodology represents a new way to design metal alloys for OER electrocatalysts or other electrocatalytic devices.
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
BIOSENSORS & BIOELECTRONICS
·
2015
·
IF 6.409
Li-Ping Mei,Jiu-Ju Feng,Liang Wu,Jia-Ying Zhou,Jian-Rong Chen,Ai-Jun Wang
Developing new nanomaterials is of key importance to improve the analytical performances of electrochemical biosensors . In this work, palladium–copper alloyed nanocages supported on reduced graphene oxide (RGO–PdCu NCs) were facilely prepared by a simple one-pot solvothermal method . A novel phenol biosensor based on laccase has been constructed for rapid detection of catachol, using RGO–PdCu NCs as electrode material . The as-developed phenol biosensor greatly enhanced the electrochemical signals for catechol . Under the optimal conditions, the biosensor has two linear ranges from 0.005 to 1.155 mM and 1.655 to 5.155 mM for catachol detection at 0.6 V, the sensitivity of 12.65 µA mM −1 and 5.51 µA mM −1 , respectively. This biosensor showed high selectivity, low detection limit, good reproducibility, and high anti-interference ability.
研究领域:
生物化学
·
材料科学
·
环境监测
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）