Catalysis Science & Technology
·
2021
·Vol. 11
·期 22
·7268-7277
·
IF 6.119
Weixiao Sun,Peng Lin,Qinghu Tang,Fangli Jing,Qiue Cao,Wenhao Fang
The synergistic effect between bimetallic nanoparticles, as well as the support effect, is particularly important for supported catalysts in heterogeneous catalysis. In this work, an AgPd/ZrO2 bimetallic catalyst was reported for the base-free aerobic oxidation of vanillyl alcohol to vanillin, a challenging transformation of an aromatic bio-alcohol into a valuable fine chemical. The crystalline structure and textural properties of ZrO2 were modulated by using different zirconium precursors and precipitants during the precipitation process. The ZrO2 obtained from zirconium nitrate and trimethylamine was found to be the most suitable support. It displayed abundant reactive oxygen species and the largest specific surface area. Then, an Ag promoter was added to the Pd/ZrO2 catalyst and the synergy between Ag and Pd was tuned by varying their ratios. The Ag0.5Pd1/ZrO2 catalyst showed an enhanced performance, i.e., 100% conversion of vanillyl alcohol and 95% selectivity to vanillin at 120 °C and 3 bar O2 within 4 h, in comparison with the Pd/ZrO2 catalyst (69% and 87%, respectively). Moreover, the vanillin productivity reached 133.0 mol mol−1 h−1, the best result reported in the literature to date. Various characterization methods demonstrated that the addition of Ag can reduce the mean size of Pd nanoparticles (4.9 nm vs. 3.8 nm), and Ag+ species were beneficial to stabilizing Pd0 species in a high fraction due to electron transfer. The reactive Pd0 sites closely interacting with the Ag promoter allowed lowering of the apparent activation energy of the reaction (27.3 vs. 37.5 kJ mol−1). In addition, the Ag0.5Pd1/ZrO2 catalyst exhibited superior stability during consecutive recycling uses owing to the strong metal–support interactions.
研究领域:
催化化学
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材料科学
·
绿色化学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2018
·
IF 11.698
Hongxia Liu,Meng Wang,Xuqiang Zhang,Jiantai Ma,Gongxuan Lu
The development of an active but cheaper catalyst is critical for efficient photocatalytic hydrogen from renewable source. In this study, we develop a high active catalyst for hydrogen evolution from formaldehyde via alloying of Pd with Ag and sensitization with a dye eosin Y (EY). The XRD, XPS, TEM and HRTEM characterizations indicate that the catalyst exhibits a core-shell structure (Ag core and Ag-Pd shell). Alloying Pd with Ag not only provides more efficient catalytic sites than single component Pd catalyst, but greatly promotes the efficient electron transfer and prolongs the lifetime of photogenerated electrons, enhances the charge separation efficiency and the photocatalytic hydrogen evolution activity significantly. The catalyst activity for hydrogen is highly dependent on the adsorption energies of HCHO and H 2 O molecules on metal surface of the alloy catalyst. Our results disclose a new route to high efficient catalyst development for solar hydrogen generation from formaldehyde.
研究领域:
材料科学
·
能源化学
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2017
·
IF 3.387
Fang Yao,Xiao Li,Chao Wan,Lixin Xu,Yue An,Mingfu Ye,Zhao Lei
Bimetallic AgPd nanoparticles with various molar ratios immobilized on graphitic carbon nitride (g-C 3 N 4 ) were successfully synthesized via a facile co-reduction approach. The powder XRD, XPS, TEM, EDX, ICP-AES and BET were employed to characterize the structure, size, composition and loading metal electronic states of the AgPd/g-C 3 N 4 catalysts. The catalytic property of as-prepared catalysts for the dehydrogenation of formic acid (FA) with sodium formate (SF) as the additive was investigated. The performance of these catalysts, as indicated by the turnover frequency (TOF), depended on the composition of the prepared catalysts. Among all the AgPd/g-C 3 N 4 catalysts tested, Ag 9 Pd 91 /g-C 3 N 4 was found to be an exceedingly high activity for decomposing FA into H 2 with TOF up to 480 h −1 at 323 K. The prepared catalyst is thus a potential candidate for triggering the widespread use of FA for H 2 storage.
研究领域:
化学
·
材料科学
·
能源研究
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2016
·Vol. 6
·期 52
·46908-46914
·
IF 3.289
Lixin Xu,Bo Jin,Jian Zhang,Dang-guo Cheng,Fengqiu Chen,Yue An,Ping Cui,Chao Wan
Bimetallic AgPd nanoparticles were successfully immobilized on graphitic carbon nitride (g-C3N4) functionalized SBA-15 for the first time by a facile co-reduction method. These catalysts were applied in the decomposition of formic acid. The dehydrogenation of formic acid is dependent on the composition of AgPd and the content of carbon nitride (CN). Among all of the AgPd/mCND/SBA-15 catalysts tested, the Ag10Pd90/0.2CND/SBA-15 catalyst exhibits highly superior performance for the decomposition of formic acid into high-quality hydrogen at 323 K with 100% hydrogen selectivity and a turnover frequency of 893 h−1, which is among the maximum values obtained at 323 K in this paper. The improved performance is a promising step towards the utilization of formic acid as a hydrogen storage material.
研究领域:
材料科学
·
催化化学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2015
·
IF 3.313
Lan Yang,Wei Luo,Gongzhen Cheng
Monodisperse trimetallic CoAgPd alloy nanoparticles (NPs) were synthesized by a controlled co-reduction of cobalt (II) acetylacetonate , silver nitrate and palladium acetylacetonate in oleylamine at 90 °C using 2-methylpyridine borane as the reducing agents. This is the first time using amine borane as the reducing agent to synthesize non-noble metal contained monodisperse trimetallic alloy NPs at relatively low temperature. The 2.8 nm monodisperse CoAgPd NPs were further assembled on graphene by a simple solution-phase self-assembly method, and tested for catalytic dehydrogenation of formic acid at room temperature . Unexpectedly, the introducing of small amount of cobalt can significantly enhance the catalytic activity and selectivity.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
ACS Omega
·
2020
·
IF 2.87
Yao Feng,Juanjuan Yin,Shufeng Liu,Yuying Wang,Bingfan Li,Tifeng Jiao
Poly(ethylene imine) (PEI) has abundant amino groups in a macromolecular chain and can be used as a graft source for metal nanocomposites, which shows excellent ability to form stable complexes with heavy metal ions. In this work, a simple and convenient method was used to make PEI into a stable hydrogel with 1-ethyl-3-(3-dimethylaminopropyl)carbodiimide-N-hydroxysuccinimide and subsequently coprecipitate with silver nitrate solution or palladium chloride solution to form metal-loaded composite hydrogels. In addition, the characterizations of composite hydrogels were investigated by scanning electron microscopy, specific surface area tests (Brunauer–Emmett–Teller), X-ray photoelectron spectroscopy, and ultraviolet spectroscopy. The properties of composite hydrogels on the catalytic reduction of 4-nitrophenol were studied. The results showed that the composite hydrogels could be easily separated from the water environment, which indicated the large-scale potential application in organic catalytic degradation and wastewater treatment.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
RSC Advances
·
2015
·Vol. 5
·期 50
·39878-39883
·
IF 3.84
Cheng Feng,Yunhui Hao,Li Zhang,Ningzhao Shang,Shutao Gao,Zhi Wang,Chun Wang
Formic acid (FA) has tremendous potential as a safe and convenient source of hydrogen for renewable energy storage, but controlled and efficient dehydrogenation of FA by a robust solid catalyst constitutes a major challenge. In this report, a metal nanoparticle functionalized zeolitic imidazolate framework (ZIF) derived N-decorated nanoporous carbon (NPC) support was fabricated and used as an efficient FA decomposition catalyst for the first time. The resultant AgPd@NPC catalyst exhibited 100% H2 selectivity and high catalytic activity (TOF = 936 h−1) toward the dehydrogenation of formic acid at 353 K. The synergetic interaction between the metal nanoparticles and NPC greatly enhances the catalytic performance of the as-prepared catalyst.
研究领域:
催化化学
·
能源材料
·
纳米材料
·
物理化学
·
氢能存储
✓ 已验证
DOI
高影响因子
Journal of the American Chemical Society
·
2017
·
IF 13.858
Xingzhong Zhu,Hang Kuen Yip,Xiaolu Zhuo,Ruibin Jiang,Jianli Chen,Xiao-Ming Zhu,Zhi Yang,Jianfang Wang
The synthesis of metal nanostructures with plasmon wavelengths beyond ∼1000 nm is strongly desired, especially for those with small sizes. Herein we report on a AgPd-tipping process on Au nanobipyramids with the resultant red plasmon shifts reaching up to ∼900 nm. The large red plasmon shifts are ascribed to the deposition of the metal at the tips of Au nanobipyramids, which is verified by electrodynamic simulations. The method has been successfully applied to Au nanobipyramids and nanorods with different longitudinal dipolar plasmon wavelengths, demonstrating that the plasmon wavelengths of these Au nanocrystals can be extended to the entire near-infrared region. Pt can also induce the tipping on Au nanobipyramids and nanorods to realize red plasmon shifts, suggesting the generality of our approach. We have further shown that the metal-tipped Au nanobipyramids possess a high photothermal conversion efficiency and good photothermal therapy performance. This study opens up a route to the construction of Au nanostructures with plasmon resonance in a broad spectral region for plasmon-enabled technological applications.
研究领域:
材料科学
·
纳米技术
·
光学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
RSC Advances
·
2016
·Vol. 6
·期 107
·105940-105947
·
IF 3.289
Daohua Sun,Pengyao Li,Bin Yang,Yan Xu,Jiale Huang,Qingbiao Li
Monodisperse AgPd nanoparticles (NPs) were successfully synthesized by coreducing silver nitrate and palladium chloride in the presence of oleylamine. Characterization techniques such as transmission electron microscopy, energy-dispersive X-ray spectroscopy, and X-ray diffraction were employed to verify the alloy nature of the obtained NPs. These AgPd NPs, supported on carbon, were found to be active catalysts for the generation of hydrogen from the methanolysis of ammonia borane at room temperature. The catalytic activity depended on the alloy composition, and the Ag30Pd70 NPs displayed the greatest activity among the tested catalysts, with a very high total turnover frequency value of 366.4 min−1 and activation energy of 37.5 kJ mol−1. In a reusability test, the Ag30Pd70/C catalyst retained 67% of its initial activity and 100% conversion after eight cycles.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
Nanoscale
·
2020
·Vol. 12
·期 5
·3469-3481
·
IF 6.895
Longfei Guo,Fuyi Chen,Tao Jin,Huazhen Liu,Nan Zhang,Yachao Jin,Qiao Wang,Quan Tang,Bowei Pan
Formate is a kind of carbon-neutral fuel that can be synthesized by electrochemical conversion of CO2, however, the generated aqueous formate electrolyte is still short of potential application. Here, formate solution is proposed to be utilized as anode fuels of direct formate fuel cells through the formate oxidation reaction (FOR), and graphene supported AgPd nanoalloys (AgPd/rGO) are prepared to catalyze the FOR. Specifically, the mass activity of the as-prepared Ag49Pd51/rGO catalyst is 4.21 A mg−1Pd and the retention activity of Ag49Pd51/rGO is 49.1% of initial activity after successive 500 cycles, which is 2.48 and 3.03 times higher than that of unsupported Ag51Pd49 nanoalloys. When increasing the positive scan limit from 0.0 to 0.8 V, the mass activity of the Ag49Pd51/rGO catalyst increases from 2.32 to 6.03 A mg−1Pd and Pd surface coverage increases from 51.87% to 62.42%, indicating the occurrence of surface reconstruction where Pd atoms migrate to the surface of AgPd nanoalloys, and less intensive reconstruction is observed in unsupported Ag51Pd49 nanoalloys, whose mass activity increases from 1.35 to 2.49 A mg−1Pd. The driving force and kinetic path are calculated for the surface reconstruction induced by the adsorption of H, O and C atoms, in the case of C atoms on graphene, the segregation energy of surface Pd atoms in the AgPd nanoalloy is −1.16 eV, and the activation energy for the migration of subsurface Pd atoms to the surface is 0.54 eV, which are lower than the segregation (0.03 eV) and activation (2.06 eV) energy on a clean alloy surface.
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
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2019
·
IF 6.361
Xian Sun,Qi Qiang,Zhiguang Yin,Zenglin Wang,Yi Ma,Chuan Zhao
Alloyed nanoparticles are promising electrocatalysts for electrochemical energy storage and conversion devices. However, syntheses of alloyed nanoparticles with controllable size and stoichiometry remain challenging. In this study, continuous, uniform and monodispersed bimetallic AgPd nanoparticles (NPs) with diameters ∼10 nm are achieved by electrochemical synthesis from quaternary ionic liquid microemulsion (ILM) for use as electrocatalysts for ethanol oxidation reaction (EOR). It is found that the ionic liquid, 1-butyl-3-methyl-imidazolium chloride ([BMIM]Cl), acts not only as a soft template and co-surfactant for the formation of micro-reactors, but also as an electrolyte for enhancing conductivity. The stoichiometry (Ag x Pd y ), size and size distribution of AgPd NPs can be accurately tuned by varying electrolyte composition , electrodeposition conditions, and ionic liquids concentrations. Attributed to the high surface area, optimal stoichiometric ratio, and strong attachment onto substrates without using organic binders, the as-deposited Ag x Pd y NPs exhibit extraordinary electrocatalytic activity and stability for EOR. It is found that the mass activity of Ag 49 Pd 51 NPs/Pt electrode reaches 3360 mA mg −1 for EOR in 1.0 M ethanol and 1.0 M KOH aqueous solution, which is much higher than commercial Pd/C catalyst (210.5 mA mg −1 ) and also the highest among state-of-the-art AgPd NPs electrocatalysts reported to date for EOR in alkaline media.
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
RSC Advances
·
2019
·Vol. 9
·期 54
·31440-31446
·
IF 3.049
Nannan Dou,Siyu Zhang,Jianying Qu
In this paper, Ag–Pd bimetallic nanoparticles uniformly distributed on reduced graphene oxide (rGO) were synthesized by redox reaction between Pd2+, Ag+and GO, and were characterized by X-ray diffractometry, field emission scanning electron microscopy, electrochemical impedance spectroscopy and thermal gravimetric analyses. A novel electrochemical sensor was constructed based on these nanocomposites using glassy carbon as a substrate. Under optimal conditions, the linear ranges were 0.50–300.00 μM for PA and 1.00–300.00 μM for 4-AP, with the detection limits of 0.23 μM for PA and 0.013 μM for 4-AP, respectively. This sensor was successfully applied to the determination of PA in pharmaceutical formulations and gave satisfactory results with a lower detection limit, wider linear range and good reproducibility.
研究领域:
分析化学
·
材料科学
·
医学检测
✓ 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）