ChemCatChem
·
2019
·Vol. 11
·期 6
·1779-1788
·
IF 4.495
Wei Zhang,Ziqiang Xiao,Jiajun Wang,Wenqin Fu,Rong Tan,Donghong Yin
Graphical Alloys of Catalysis ! Synergistic effect in Au−Pd alloy catalysts enhanced selective aerobic oxidation of alcohols using air at atmospheric pressure in water. A series of bimetallic Au−Pd alloy nanoparticles (NPs) with varied Au/Pd molar ratios was supported on Gamma-alumina (γ-Al 2 O 3 ) surface through the co-impregnation-reduction method using HAuCl 4 and PdCl 2 as metal precursors. Characterization results suggested the high dispersion of Au−Pd alloy NPs, as well as the interplay between the two compositions. Benefitting from the synergistic effects of Au−Pd alloying, the bimetallic Au-Pd x @γ-Al 2 O 3 catalysts were highly efficient for selective aerobic oxidation of various alcohols either aromatic or aliphatic in water using air at atmospheric pressure as a sole oxidant without the need for any cocatalyst. Quantitative yields of corresponding aldehydes or ketones were achieved over Au-Pd 1.2 @γ-Al 2 O 3 within 2 h, whereas pure Au@γ-Al 2 O 3 or Pd@γ-Al 2 O 3 was far less efficient. More importantly, the “alloying effect” appeared to stabilize the bimetallic NPs against aggregation and poisoning, which made the Au-Pd x @γ-Al 2 O 3 more stable and reusable in the aerobic oxidation of alcohols.
研究领域:
化学
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催化材料科学
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产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Yajie Guo,Fuxian Zheng,Ting Wang,Xinyang Liu,Xiaotan Tian,Konggang Qu,Lei Wang,Rui Li,Wenjun Kang,Zongge Li,Haibo Li
Palladium (Pd)-transition metal alloys have the potential to regulate the intermediate surface adsorption strength in oxygen reduction reactions (ORR), making them a promising substitute for platinum-based catalysts. Nonetheless, prolonged electrochemical cycling can lead to the depletion of transition metals, resulting in structural degradation and poor durability. Herein, the synthesis of alloy catalysts (Pd25%Te75%) containing Pd and the metalloid tellurium (Te) through a one-step reduction method is reported. Characterizations of powder X-ray photoelectron spectroscopy, X-ray diffraction, and high-resolution transmission electron microscopy demonstrated both uniform dispersion and strong binding force of elements within the PdTe alloy, along with providing crystallographic details of associated compounds. Based on density functional theory calculations, PdTe had a more negative d-band center than that of pure Pd, which reduces the adsorption capacity between active sites and intermediates in the ORR, and therefore enhances reaction kinetics. The Pd25%Te75% exhibited excellent ORR activity, and its onset and half-wave potentials were ∼0.98 and ∼0.90 V, respectively, at 1600 rpm within the O2-saturated 1.0 M KOH. Significantly, accelerated durability tests achieved exceptional stability, and half-wave potential just decayed by 4 mV after 30000 consecutive cycles. Moreover, this study aims to promote the preparation of Pd and metalloid alloys for other energy conversion applications.
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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产品关联
DOI
PubMed
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
JOURNAL OF POWER SOURCES
·
2025
·
IF 7.9
Lingling Li,Yingliang Feng,An Pei,Lihua Zhu,Weizhen Wang,Guang Li,Chengxiu Huang,Zhiqing Yang,Hengqiang Ye
Different atomic ratios of PtPd alloy nanoparticles (NPs) supported on carbon doping with nitrogen-NC (Pt x Pd y /NC) are successfully prepared to simultaneously enhance hydrogen evolution reaction (HER) and methanol oxidation reaction (MOR), in which Pt 5 Pd 5 /NC with an atomic ratio of 5:5 has the best performance. Pt 5 Pd 5 /NC exhibits a significantly reduced HER overpotential (12 mV@10 mA cm −2 ) and the mass activity (MA) for MOR is up to 6.85 A mg −1 PtPd , 11.61 and 34.25 times higher than that of commercial Pt/C (Pt/C-JM) and commercial Pd/C (Pd/C-JM), respectively. Remarkably, coupling boosted HER on the cathode with accelerated MOR on the anode, efficient H 2 generation is achieved. This two-electrode flow cell only requires a cell voltage of 1.100 V at 100 mA cm −2 and can be stably operated for >300 h at 1.960 V with impressive long-life stability. Such performance even outperforms that of (IrO 2 ) OER‖HER (Pt/C-JM) cell. Electrochemical in-situ Fourier transform infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS) analysis show that electronic effect is formed between N and PtPd and can oxidize the intermediate HCOO - at a lower potential (0.300 V), promote the desorption of the toxic intermediates and improve the catalytic property.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
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2021
·
IF 7.92
Zhi-Feng Jiao,Ya-Ming Tian,Xiao-Ning Guo,Udo Radius,Holger Braunschweig,Todd B. Marder,Xiang-Yun Guo
A highly efficient photocatalytic protocol for borylation of alkyl bromides and chlorides with graphene supported Cu/Pd alloy nanoparticles as a heterogeneous catalyst is reported. This photocatalytic system operates with visible light in air, providing a wide range of primary and secondary alkyl halides with B 2 pin 2 or B 2 neop 2 in high yields at low temperatures, thereby demonstrating its broad utility and functional group tolerance. The high performance is attributed to a synergistic effect of localized surface plasmon resonance (LSPR) of Cu and charge transfer from Cu to Pd due to the alloy surface charge heterogeneity. Transfer of energetic electrons from Pd to electrophilic alkyl halides lead to the formation of the alkyl radicals, which quickly react with a nucleophilic adduct of a diboron compound with base adsorbed on the positively charged Cu sites to form the corresponding borylation product.
研究领域:
有机化学
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材料科学
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催化化学
✓ 已验证
DOI
高影响因子
ANALYST
·
2022
·Vol. 147
·期 24
·5655-5662
·
IF 5.227
Ying Zhou,Ruichun Li,Guomei Zhang,Yan Zhang,Caihong Zhang,Shaomin Shuang
Metal–organic frameworks (MOFs) have emerged as interesting nanomaterials owing to their large surface area, high porosity, tunable pore architecture and easy functionalization. However, an inferior electrical conductivity hinders their application in electrochemical sensing. In this paper, gold–palladium alloy/UiO-66-NH2/graphene (AuPd/UiO-66-NH2/GN) composites were synthesized by loading alloys on the surfaces of MOFs and then attaching them to the graphene surface. The addition of metal nanoparticles and graphene enhanced the electron transfer ability of MOFs. Then, composites were used to modify a glassy carbon electrode (GCE) to construct a sensitive dopamine (DA) electrochemical sensor. The developed sensor manifested two linear relationships in lower concentration ranges and in higher concentration ranges with a 0.21 × 10−6 mol L−1 low detection limit (3σ/k) under optimal conditions. The results certified that the constructed sensor had high selectivity, excellent reproducibility and good stability, and had been used successfully for DA detection in actual human serum samples.
研究领域:
材料科学
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分析化学
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生物医学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
FUEL
·
2024
·
IF 6.7
Yuyang Cao,Shilong Yang,Yuting Liu,Xingyu Liu,Yue Li,Xiucheng Zheng,Zhikun Peng,Pu Liu
At present, controllable producing hydrogen from the catalytic hydrolysis of ammonia borane (AB, NH 3 BH 3 ) is very meaningful and challenging. Therefore, developing an effective catalyst for the reaction, clarifying its catalytic mechanism, and realizing controllable hydrogen release are extremely indispensable. In this work, RuPd nanoalloys are evenly confined by the agricultural waste wheat straw-derived carbon (denoted as WSC) with a micropore-dominant porous structure and plentiful N/O doping. Attributing to the particular support effect of WSC and the interesting RuPd alloy effect, the as-prepared bimetallic catalysts provide encouraging catalytic performance in AB hydrolysis. Catalyzed by the optimal Ru 0.50 Pd 0.50 @WSC, the turnover frequency (TOF) and hydrogen evolution rate are 214.5 min −1 and 50800 mL min −1 g −1 , respectively, and the apparent activation energy is only 23.2 kJ mol −1 . Moreover, introducing proper NaOH (1.5 M) further accelerates hydrogen release (TOF = 502.8 min −1 , specific rate = 119100 mL min −1 g −1 ). The isotope experiments depict a kinetic isotope effect of 2.85, evidencing the vital role of the hydrogen–oxygen bond scission in this catalytic reaction. More importantly, benefitting from the difference in adsorption energy and strong coordination ability, the “on–off” control for the hydrolysis of AB over Ru 0.50 Pd 0.50 @WSC can be realized with the Zn 2+ /EDTA 2- system. This study provides an attractive metal alloy catalyst and some insights for the controllable hydrolysis of AB.
研究领域:
化学
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材料科学
·
催化反应
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2017
·
IF 7.504
Jin Wang,Peina Zhang,Yujiao Xiahou,Dayang Wang,Haibing Xia,Helmuth Möhwald
The present work introduces a new way to prepare Au–Pd alloy nanowire networks (NWNs) via deposition of Pd atoms onto Au nanowires in reaction media at room temperature without the aid of additional reducing agents. Thanks to their excellent colloidal stability in water as well as in ethanol, the resulting NWNs can be utilized to produce composite thin films with Nafion (perfluorinated sulfonic acid) with dimensions above dozens of square centimeters by means of solution casting on the glass substrate. Most importantly, these films can be easily transferred onto different solid substrates by lift-off technology. Moreover, the resulting Au–Pd alloy NWNs can also be easily and thoroughly loaded into macroscopic carbon fiber cloth (CFC). Both the Au–Pd alloy NWN/Nafion composite film and the Au–Pd alloy NWN-loaded CFC can be used as flexible electrodes for electrocatalysis of ethanol oxidation, with electrocatalytic performance at different distorted states superior by 2 orders of magnitude to those reported in the literature (e.g., commercial Pd/C catalysts and Pd-based nanostructured catalysts). This work opens new possibilities for the large-scale manufacturing of electrodes for fuel cells.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-18
·
IF 14.7
Meng Xiangqin,Fan Huizhen,Chen Lei,He Jiuyang,Hong Chaoyi,Xie Jiaying,Hou Yinyin,Wang Kaidi,Gao Xingfa,Gao Lizeng,Yan Xiyun,Fan Kelong
Developing strategies that emulate the killing mechanism of neutrophils, which involves the enzymatic cascade of superoxide dismutase (SOD) and myeloperoxidase (MPO), shows potential as a viable approach for cancer therapy. Nonetheless, utilizing natural enzymes as therapeutics is hindered by various challenges. While nanozymes have emerged for cancer treatment, developing SOD-MPO cascade in one nanozyme remains a challenge. Here, we develop nanozymes possessing both SOD- and MPO-like activities through alloying Au and Pd, which exhibits the highest cascade activity when the ratio of Au and Pd is 1:3, attributing to the high d-band center and adsorption energy for superoxide anions, as determined through theoretical calculations. The Au 1 Pd 3 alloy nanozymes exhibit excellent tumor therapeutic performance and safety in female tumor-bearing mice, with safety attributed to their tumor-specific killing ability and renal clearance ability caused by ultrasmall size. Together, this work develops ultrasmall AuPd alloy nanozymes that mimic neutrophil enzymatic cascades for catalytic treatment of tumors.
研究领域:
生物医学工程
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肿瘤学
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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
·
2019
·
IF 8.456
Yang Yang,Minghua Tian,Qiaoxia Li,Yulin Min,Qunjie Xu,Shaowei Chen
Bimetallic nanostructures represent effective electrocatalysts toward a number of important reactions. In the present study, carbon-supported palladium–tungsten alloy nanoparticles with a quasi-tungsten core@palladium shell structure (W@Pd/C) were synthesized by a galvanic replacement reaction of amorphous tungsten nanoparticles with Pd(II) at different temperatures (0, 25, and 50 °C), and exhibited apparent electrocatalytic activity toward ethanol oxidation reaction (EOR). When the sample was prepared at 0 °C, large amorphous tungsten nanoparticles were etched off and much smaller W@Pd nanoparticles were formed and dispersed rather evenly on the carbon surface whereas at higher reaction temperatures (25 and 50 °C), the W@Pd nanoparticles became agglomerated. The structures of the obtained samples were characterized by a range of experimental tools, including (scanning) transmission electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy, and electrochemical methods. Among the series, the W@Pd/C sample prepared at 0 °C was observed to exhibit the best EOR performance, with a mass activity (9535.5 mA mgPd–1) over three times better than that of commercial Pd/C and markedly enhanced stability.
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
APPLIED CATALYSIS A-GENERAL
·
2023
·
IF 5.5
Shuang Wang,Cheng Li,Rujie Shang,Huihui Zhang,Kehui Qi,Yao Yao,Chunyan Yu,Qing Liu,Guorui Li,Shitao Yu,Lu Li
Producing vanillin from lignin model compounds in an elegant and efficient manner is a focus of chemical utilization in lignocellulosic biomass. The facile synthesis of a cobalt-palladium bimetallic alloy anchored on activated carbon (Co-Pd/C), which excels in the selective oxidation of the lignin model compound 4-methylguaiacol to vanillin, is reported here. The characterization results of Co-Pd/C indicate that the catalysts enhance the catalytic efficiency by forming a cobalt-palladium alloy to modulate the number of d-band cavities and influence the O 2 adsorption. Meanwhile, the synergistic effect between the alloys causes the Co-Pd/C catalyst exhibits good activity and stability in cycling experiments. A series of controlled experiments offer insight into the mechanism of catalytic generation of vanillin from 4-methylguaiacol. This work opens a new opportunity for achieving the valuable aromatic products from lignin.
研究领域:
生物质化学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
Nanoscale
·
2015
·Vol. 7
·期 13
·5699-5705
·
IF 7.394
Jing-Jing Lv,Li-Ping Mei,Xuexiang Weng,Ai-Jun Wang,Li-Li Chen,Xiang-Feng Liu,Jiu-Ju Feng
A facile one-pot solvothermal method was developed for the fabrication of well-defined three-dimensional highly branched Pt–Pd alloyed multipods, using ethylene glycol as a solvent and a reducing agent, along with N-methylimidazole as a structure-directing agent, without any seed, template, or surfactant. The as-prepared nanocrystals exhibited a relatively large electrochemically active surface area, improved electrocatalytic activity and superior stability for ethylene glycol oxidation in alkaline media, compared with commercial Pt black and Pd black, making them promising electrocatalysts in fuel cells.
研究领域:
材料科学
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电化学
✓ 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）