ELECTROCHIMICA ACTA
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2014
·
IF 4.086
Jie-Ning Zheng,Ming Zhang,Fang-Fang Li,Shan-Shan Li,Ai-Jun Wang,Jiu-Ju Feng
In this report, a simple and rapid method was developed for the large-scaled synthesis of well-defined Pd nanochains based on one-pot wet-chemical reduction of PdCl 2 with KBH 4 , with the assistance of octylphenoxypolyethoxyethanol (OP-10) as a growth directing agent. The concentration of OP-10, the strength of a reducing agent and its amount, and the reaction temperature were demonstrated essential for preparation of the Pd nanocrystals. Furthermore, the as-prepared Pd nanochains exhibited a higher electrochemically active surface area and the enhanced electrocatalytic performance for formic acid oxidation in acid media, compared with the Pd nanoparticles.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2013
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IF 2.39
Zhang-Ying Lv,Yao Fei,Wan-Yi Chen,Yan-Fei Tan,Chao-Qun Sun,Jian-Rong Chen,Ai-Jun Wang,Jiu-Ju Feng
In this report, a simple, facile, controllable, and green one-step electrochemical co-deposition method was developed for the preparation of hierarchical wheat-like Au–Pd heterostructures on a glassy carbon electrode (GCE) without any template or surfactant, only using l -glutamic acid as a growth directing agent. The control experiments associated with the applied potential, the molar ratio of HAuCl 4 to PdCl 2 , electrodeposition time, and concentration of l -glutamic acid were investigated in details. Meanwhile, the electrochemical experiments demonstrate the superior electrocatalytic activity of the Au–Pd heterostructures toward methanol oxidation, achieving a maximum catalytic current density of 45.8 mA cm −2 in the presence of 0.5 M methanol, much larger than those on pure Au (5.4 mA cm −2 ) or Pd (25.0 mA cm −2 ) under the same conditions.
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JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL
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2015
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IF 3.615
Yansheng Liu,Bo Qiao,Xinlin Li,Xuanduong Le,Wei Zhang,Jiantai Ma
Palladium metal nanoparticles have been applied to hydrodechlorination of chlorophenols in contaminated water using H 2 as a clean and sustainable reductant. However, there are two major challenges to widespread technology adoption which are the activity loss caused by nanoparticle aggregation and the difficulty of nanoparticle recovery. In this study, a synthesis of a core-shell structured catalyst with encapsulated Pd nanoparticles has been given and whose catalytic activity has been tested in hydrodechlorination of chlorophenols under 1 atm H 2 at room temperature. The catalyst material consists of a nonporous silica core decorated with Pd nanoparticles that are further encapsulated within an ordered mesoporous silica shell. Well-defined mesopores (2.4 nm) provide a physical barrier to prevent Pd nanoparticle (∼10 nm) movement, aggregation and detachment from the support into water. Compared with some supported Pd catalysts such as Pd/AC and Pd/Al 2 O 3, SiO 2 /Pd@m-SiO 2 exhibits higher catalytic performance. After 5 times of recycling, catalytic activity of SiO 2 /Pd@m-SiO 2 reduces slightly and this result confirms the good recyclability of SiO 2 /Pd@m-SiO 2 . The function of the mesoporous shell, preventing aggregation of active nanoparticles, suggests a promising general strategy of using metal nanoparticle catalysts for water purification and related aqueous-phase applications.
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JOURNAL OF THE ENERGY INSTITUTE
·
2017
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IF 3.204
Qifu Huang,Wenzhi Li,Qizhao Lin,Xusheng Zheng,Haibin Pan,Dong Pi,Chunyu Shao,Chao Hu,Haitao Zhang
In this paper, the catalyst of Pd–NiCo 2 O 4 /SiO 2 was prepared and applied to the catalytic combustion of lean methane. Pd and NiCo 2 O 4 nanoparticles were uniformly distributed on the SiO 2 support, so that every Pd or NiCo 2 O 4 nanoparticle was separated from each other by another component. Comparing with Co 3 O 4 /SiO 2 , NiCo 2 O 4 /SiO 2 , Pd–Co 3 O 4 /SiO 2 and Pd#NiCo 2 O 4 /SiO 2 (catalysts without uniform distribution of Pd and NiCo 2 O 4 nanoparticles), Pd–NiCo 2 O 4 /SiO 2 had the highest catalytic activity in the catalytic combustion of lean methane, with a methane total conversion temperature at 378 °C. In addition, the high activity did not decrease during the long time reaction, which showed good thermal stability . TEM and BET results showed that the nanoparticle sizes of Pd and NiCo 2 O 4 were very small. The XRD patterns indicated that the Pd nanoparticles were highly dispersed on the surface of SiO 2 . The XPS spectra demonstrated the formation of NiCO 2 O 4 , the presence of enough active oxygen species on the catalyst surface and the high ratio of PdO/Pd 0 . The enhanced influence of Ni introduction was also proved by comparison tests. All these results indicated that the high catalytic activity of Pd–NiCo 2 O 4 /SiO 2 mainly comes from the nanoparticle distribution and the Ni cation enhancement.
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Catalysts
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2015
·Vol. 5
·期 3
·1388-1398
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IF 2
Long-Long Wang,Xiao-Lu Cao,Ya-Jun Wang,Qiao-Xia Li
The newly proposed mimetic underpotential deposition (MUPD) technique was extended to modify Pd surfaces with Sb through immersing a Pd film electrode or dispersing Pd/C powder in a Sb(III)-containing solution blended with ascorbic acid (AA). The introduction of AA shifts down the open circuit potential of Pd substrate available to achieve suitable Sb modification. The electrocatalytic activity and long-term stability towards HCOOH electrooxidation of the Sb modified Pd surfaces (film electrode or powder catalyst) by MUPD is superior than that of unmodified Pd and Sb modified Pd surfaces by conventional UPD method. The enhancement of electrocatalytic performance is due to the third body effect and electronic effect, as well as bi-functional mechanism induced by Sb modification which result in increased resistance against CO poisoning.Keywords:formic acid oxidation;palladium;Sb modification;mimetic underpotential deposition
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APPLIED SURFACE SCIENCE
·
2024
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IF 6.3
Hehe Qian,Yuetan Su,Shu Yan,Wenjun Fang,Kun Yang,Xiaole Weng
Electrocatalytic hydrodechlorination (EHDC) emerges as a promising technology for remediating chlorinated organic pollutants, garnering considerable attention. However, the long-term performance evolution of EHDC, specifically its size-dependent aspect, remains relatively unexplored. This work aims to address this gap by examining Pd nanocubes with controlled sizes of 7.2 nm for Pd Cube-S, 10.6 nm for Pd Cube-M, and 14.7 nm for Pd Cube-L. The specific activity and electrochemical turnover frequency (TOF) of these Pd cubes increased with particle size, a pattern that is inverse to the trend of mass activity. Although Pd Cube-S initially demonstrated heightened EHDC efficiency, a long-term examination over multiple EHDC cycles revealed that Pd Cube-L exhibited escalating mass activity (from 2.10 to 3.11 min −1 g −1 after 5 cycles) and maintained stability over 180 h of continuous electrolysis. This phenomenon arose from structural reorganization of Pd cubes occurring during the EHDC cycles, leading to an expansion of the electrochemically specific surface area. Such structural reorganization brought about more enhancements in large-sized Pd cubes, whereas Pd Cube-S suffered more from particle agglomeration. Consequently, by fine-tuning the particle size, this work provided valuable insights into the long-term EHDC process, offering practical implications for enhancing the durability of Pd nanocatalysts.
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CHEMISTRY OF MATERIALS
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2024
·
IF 7.2
Shikai Liu,Chuqiao Shi,Chaokai Xu,Haichuan Zhang,Wenqi Li,Valentín Briega-Martos,Qian He,Yimo Han,Yao Yang
CO2 reduction reaction (CO2RR) facilitates the sustainable synthesis of fuels and chemicals. Although copper (Cu) enables CO2-to-multicarbon product (C2+) conversion, Cu-based electrocatalysts, particularly nanocatalysts, face challenges in poor selectivity and stability owing to the highly dynamic nature of Cu atoms under reaction conditions. Core–shell structures present a promising approach to address these issues by modulating the Cu overlayer–substrate interactions with atomic-level precision. Here, we report on Pd@Cu core–shell structures with atomically thin and nanometer-thick Cu overlayers on single-crystal Pd nanocubes with {100} facets promoting the CO2-to-C2+ conversion. The microstructures and surface compositions at the atomically sharp Pd/Cu interface were investigated by atomic-scale scanning transmission electron microscopy (STEM) imaging and electron energy-loss spectroscopy (EELS). Our results reveal that atomic-layer Cu epitaxially grows on Pd and adapts to the lattice of the Pd substrate. The reaction-driven migration of atomic-layer Cu is effectively suppressed on Pd due to the strong Cu–Pd interaction. While Pd only reduces CO2 to C1 products, atomic-layer Cu on Pd can initiate the C2+ production during the CO2RR. Thick Cu overlayers (∼15 nm) on Pd further enhance the C2+ faradaic efficiency while undergoing significant structural reconstruction, with only the 2–3 nm Cu layers near the Pd surface remaining stable and resistant to Cu migration after the CO2RR. We anticipate that Pd@Cu core–shell structures with intermediate Cu shell thickness hold significant potential for enhancing C2+ selectivity while maintaining high stability of nanocatalysts for CO2 reduction to liquid fuels.
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SENSORS
·
2024
·Vol. 24
·期 7
·2110
·
IF 3.4
Yinfeng Shen,Yiping Liu,Chao Fan,Qudong Wang,Ming Li,Zhi Yang,Liming Gao
The mature processes of metal oxide semiconductors (MOS) have attracted considerable interest. However, the low sensitivity of metal oxide semiconductor gas sensors is still challenging, and constrains its practical applications. Bimetallic nanoparticles are of interest owing to their excellent catalytic properties. This excellent feature of bimetallic nanoparticles can solve the problems existing in MOS gas sensors, such as the low response, high operating temperature and slow response time. To enhance acetone sensing performance, we successfully synthesized Au-Pd/ZnO nanorods. In this work, we discovered that Au-Pd nanoparticles modified on ZnO nanorods can remarkably enhance sensor response. The Au-Pd/ZnO gas sensor has long-term stability and an excellent response/recovery process. This excellent sensing performance is attributed to the synergistic catalytic effect of bimetallic AuPd nanoparticles. Moreover, the electronic and chemical sensitization of noble metals also makes a great contribution. This work presents a simple method for preparing Au-Pd/ZnO nanorods and provides a new solution for the detection of acetone based on metal oxide semiconductor.
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PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
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2024
·Vol. 48
·期 26
·11794-11801
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IF 2.7
Mingming Du,Anxian Peng,Hongyue Liu,Qiyun Li,Likai Dai,Zheng Fang,Ganning Zeng,Huimei Chen,Rongjun Yan
The photocatalytic conversion of endless solar energy into storable and usable chemical energy, such as photocatalytic hydrogen peroxide production, is promising and attractive. However, a satisfactory hydrogen peroxide yield has not been achieved using photocatalysts due to the rapid recombination of photoexcited carriers and the rapid decomposition of H2O2. Herein, a polymer polyethyleneimine (PEI)-assisted Pd metal loading BiOCl nanosheet photocatalyst (Pd/PEI/BOC) is designed to achieve higher photocatalytic activity. Experimental results show that compared to the Pd/BOC catalyst with a Pd loading of only 0.26 wt%, the Pd/PEI/BOC catalyst can achieve a higher Pd loading of 0.45 wt%, which is due to the obvious shifting of the isoelectric point (IEP) of BiOCl from the pH value of 4.1 to 8.4 in the presence of PEI, leading to enhanced immobilization. Furthermore, H2O2 decomposed more slowly for the Pd/BOC catalyst modified by PEI. In addition, Pd can significantly enhance the separation of electrons–holes and light absorption range, especially for visible light. Therefore, under simulated sunlight, this Pd/PEI/BOC catalyst displayed a higher H2O2 production ability of 3700.23 μmol g−1 h−1.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-10
·
IF 14.7
Fang Cao,Xu Chang,Zhang Wei,Zhou Meng,Tan Dong,Qian Lixia,Hu Daqiao,Jin Shan,Zhu Manzhou
Dual emission (DE) in nanoclusters (NCs) is considerably significant in the research and application of ratiometric sensing, bioimaging, and novel optoelectronic devices. Exploring the DE mechanism in open-shell NCs with doublet or quartet emissions remains challenging because synthesizing open-shell NCs is difficult due to their inherent instability. Here, we synthesize two dual-emissive M 1 Ag 13 (PFBT) 6 (TPP) 7 (M = Pt, Pd; PFBT = pentafluorobenzenethiol; TPP = triphenylphosphine) NCs with a 7-electron open-shell configuration to reveal the DE mechanism. Both NCs comprise a crown-like M 1 Ag 11 kernel with Pt or Pd in the center surrounded by five PPh 3 ligands and two Ag(SR) 3 (PPh 3 ) motifs. The combined experimental and theoretical studies revealed the origin of DE in Pt 1 Ag 13 and Pd 1 Ag 13 . Specifically, the high-energy visible emission and the low-energy near-infrared emission arise from two distinct quartet excited states: the core-shell charge transfer and core-based states, respectively. Moreover, PFBT ligands are found to play an important role in the existence of DE, as its low-lying π * levels result in energetically accessible core-shell transitions. This novel report on the dual-quartet phosphorescent emission in NCs with an open-shell electronic configuration advances insights into the origin of dual-emissive NCs and promotes their potential application in magnetoluminescence and novel optoelectronic devices.
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APPLIED ORGANOMETALLIC CHEMISTRY
·
2024
·
IF 3.7
Xiaohua Zhao,Xiaoxiao Liu,Xiang Liu,Weiyi Li,Ping Wang
Integration of localized surface plasmon resonance (LSPR) metallic nanocrystals into photocatalysis is an intriguing approach for light-driven organic transformations. However, uncertain direction of hot carriers is a grand challenge, which fails to take full advantage of the LSPR excitation. In this work, core–shell gold@ceria nanosphere–supported segregated palladium species (Au@CeO 2 –Pd) have developed to steer the light absorption capability and charge carrier migration. Under simulated solar light irradiation, the core–shell–satellite Au@CeO 2 –Pd exhibited efficient light harvesting and colossal activity in the Suzuki coupling reaction. The plasmon-induced hot electrons overpassed the Schottky barrier at the Au@CeO 2 interfaces and migrated from Au core to CeO 2 shell accordingly. Subsequently, the photogenerated electrons and hot electrons migrated from Au@CeO 2 core–shells to Pd, which acted as an electron acceptor. Detailed photocatalytic mechanism studies revealed that both photoexcited electrons and holes were the main active species involved in the photocatalytic Suzuki coupling reaction process. In particular, the diphenyl yield over Au@CeO 2 –Pd catalyst was ~1.7 times higher than that of core–shell–satellite Au@SiO 2 –Pd, where a 19-nm-thick SiO 2 shell was introduced to prevent the migration of hot electrons. This distinctly certified that the hot electrons transfer in the core–shell–satellite Au@CeO 2 –Pd under illumination played an important role to drive Suzuki reaction. Overall, this design of core–shell–satellite Au@CeO 2 –Pd plasmonic photocatalyst has the potential in the field of photo-driven organic transformations.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Huizhen Sun,Xiuhua Chen,Shaoyuan Li,Wenhui Ma,Xiumin Chen,Dandan Wu,Kaixin Fu,Mingjun Xiao,Ming Wen
Developing efficient and selective recovery of Pd(II) adsorbents is crucial for addressing environmental pollution issues. Among them, covalent organic framework (COF) and metal organic framework (MOF) composites due to the multi-site functional groups are expected to exhibit excellent Pd(II) adsorption. However, the design and preparation of COF and MOF composite adsorbents for highly efficient adsorption of heavy metal Pd(II) still face many challenges. Herein, we constructed a series of novel core–shell structure UiO-66-NH 2 @TAP-COF (denoted as M@C) adsorbents (M@C-X, X = 1–5, representing different MOF doses) by Schiff base reaction and applied in the adsorption of Pd(II). The findings indicated that the M@C-3 exhibited ultra-high adsorption performance, reaching a capacity of 2134.1 mg/g, and displayed excellent selectivity, making it the best among similar materials. Experimental data and density functional theory (DFT) calculations revealed that the efficient and selective adsorption of Pd(II) is attributed to coordination interaction and strong electrostatic between Pd(II) and the abundant N and O groups in M@C. This work demonstrates the significant potential of the constructed core–shell M@C composites for the efficient and selective recovery of precious metal Pd(II).
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