GREEN CHEMISTRY
·
2022
·Vol. 24
·期 4
·1570-1577
·
IF 11.034
Ruixue Yangcheng,Jiansu Ran,Zhaohui Liu,Yuntong Cui,Jianjian Wang
Efficient production of high value-added chemicals and biofuels via low-temperature chemoselective HDO of lignin derivatives in water is still a challenge. Here, we construct a low-cost, active and stable Pd/PCE catalyst using phosphoric acid-modified commercial Celite (PCE) as the support, and this catalyst exhibits excellent activity in low-temperature HDO of vanillin as well as other lignin derivatives in water. The superior catalytic performance is due to the presence of P species on the surface of Pd/PCE, accelerating the selective conversion of the intermediate into the final product. Detailed experimental and mechanistic studies reveal that the rapid conversion of the intermediate to the final product proceeds via a free-radical process in an interfacial microenvironment created by intimate interacting between the P species and Pd NPs. The insights of this work provide a new low-cost catalytic system for efficient production of valuable chemicals and future biofuels from lignin derivatives.
研究领域:
化学工程
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
RARE METALS
·
2020
·Vol. 39
·期 12
·1473-1482
·
IF 2.161
Feng Shao-Ping,Huang Kun
Abstract Separation of palladium (Pd) and platinum (Pt) by solvent extraction is difficult because of their extremely similar physicochemical properties. Development of new extractants with a high extraction efficiency and excellent separation selectivity is the primary focus for enhancing the separation of Pd and Pt by solvent extraction. In this study, a new extractant, 2-((2-methoxyethyl)thio)-1H-benzimidazole (MOBI), which contains N, S, and O atoms, was synthesized and used to separate Pd(II) and Pt(IV) from a hydrochloric acid aqueous solution. The experimental results revealed that Pd(II) and Pt(IV) were effectively separated under the optimal conditions: MOBI concentration of 0.005 mol·L −1 , HCl concentration of 0.2 mol·L −1 , organic/aqueous (O/A) phase ratio of 1.0, and contact time of 15 min. The separation coefficient between Pd(II) and Pt(IV) was 1246.40, which indicates that MOBI has a higher selectivity for Pd(II) than Pt(IV). In addition, the mechanism of coordination between Pd(II) and MOBI was demonstrated through the slope method, Fourier transform infrared spectroscopy (FTIR), hydrogen-1 nuclear magnetic resonance spectroscopy ( 1 H NMR), and carbon-13 nuclear magnetic resonance spectroscopy ( 13 C NMR). The results revealed that MOBI could coordinate with Pd(II) via the N atom in the benzimidazole ring of MOBI molecules to form [Pd(MOBI) 2 Cl 2 ] (O) . Graphic abstract
研究领域:
化学
·
材料科学
✓ 已验证
DOI
高影响因子
Nanomaterials
·
2022
·Vol. 12
·期 11
·1890
·
IF 5.719
Xiaogang Liu,Wenjie Chen,Xin Zhang
The exploitation of highly efficient and stable hydrogen generation from chemical storage of formaldehyde (FA) is of great significance to the sustainable development of the future. Moreover, developing an accurate, rapid, reliable, and cost-effective catalyst for electrochemical detection of FA in solution is appealing. Herein, we report rational construction of Pd nanoparticles decorated reduced graphene oxides (Pd/rGO) nanohybrids not only as robust catalysts to produce hydrogen from alkaline FA solution and but also electrocatalysts for electrochemical detection of FA. By optimizing the reaction parameters including FA concentration, NaOH concentration and reaction temperature, Pd/rGO with Pd loading of 0.5 wt% could exhibit a high hydrogen production rate of 272 mL g−1min−1at room temperature of 25 °C, which is 3.2 times that of conventional Pd NPs. In addition, as-prepared Pd/rGO nanohybrids modified glassy carbon (GC) electrodes are used as FA-detected electrochemical sensors. A sensitive oxidation peak with a current density of 8.38 mA/cm2was observed at 0.12 V (vs. Ag/AgCl) in 0.5 M NaOH containing 10 mM FA over Pd/rGO catalysts with Pd loading of 0.5 wt%. The results showed the prepared Pd/rGO nanocatalyst not only exhibited efficient and stable hydrogen production from alkaline FA solution but also had good electrocatalytic properties with respect to formaldehyde electrooxidation as a result of the synergistic effect of Pd NPs and rGO nanosheets.Keywords:palladium;graphene;hydrogen production;formaldehyde detection
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2021
·
IF 9.028
Weiting Yu,He Jiang,Jinhui Fang,Shuang Song
Reducing the Pd loading on electrodes is critical in the electrocatalytic hydrodechlorination (EHDC) of chlorinated organic compounds (COCs). The EHDC reaction of COCs on Pd involves three steps: H* formation, H* adsorption, and dechlorination. It has been established that the initial hydrogen evolution reaction (HER) occurs on Pd0 and the dechlorination steps occur on Pd2+. A strategy is proposed to design new electrodes by adding a reducible HER-active interlayer to replace Pd0, fulfilling the responsibility of producing hydrogen, and to facilitate the formation of more Pd2+ for following C–Cl bond cleavage. Keeping the atomic hydrogen adsorption energy on the Pd/interlayer similar to that on pure Pd is also necessary for H* adsorption as well as to maintain a high EHDC activity. For the first time, the NiCo2O4-interlayer-modified Pd/Ni-foam electrode was applied in the EHDC of COCs, which enhanced the EHDC efficiency to 100% within 90 min and reduced 88.6% of Pd consumption. The Pd/NiCo2O4/Ni-foam electrode with enhanced EHDC activity was also observed with almost 100% product selectivity and good stability. A synergistic mechanism is proposed for the enhanced EHDC activity on the Pd/NiCo2O4/Ni-foam. This work offers a simple and useful strategy to design robust electrocatalysts for the EHDC of COCs.
研究领域:
化学
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环境科学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
HYDROMETALLURGY
·
2023
·
IF 4.7
Qian Xiao,Xueyu Wang,Lianjun Song,Fengfeng Li,Qiuju Li,Lanlan He,Zhen Shen,Fangxiang Luo,Songdong Ding
The increasing demand and limited natural resources for rare precious metal palladium render its separation and recovery from secondary sources such as acidic nuclear liquid waste greatly interesting. Herein, a novel Et-Tol-DAPhen extraction resin was prepared by impregnating Amberlite XAD-7 resin with a phenanthroline-derived diamide extractant N , N ′-diethyl- N , N ′-ditolyl-2,9-diamide-1,10-phenanthroline (Et-Tol-DAPhen), and the adsorption behavior of this new extraction resin towards Pd 2+ in HNO 3 solution was investigated through the batch and column experiments. The Et-Tol-DAPhen extraction resin exhibited strong adsorbability, high adsorption capacity, excellent selectivity and good reusability for Pd 2+ in highly acidic HNO 3 solution. In addition, the pseudo-second-order and Langmuir models were applied to understand the adsorption process of Pd 2+ on Et-Tol-DAPhen extraction resin, respectively. It demonstrated the characteristics of a uniform single-layer chemisorption . The maximum uptake capacity could reach as high as 74.6 mg g − 1 for Pd 2+ in 3.0 mol/L HNO 3 solution which is much higher than most adsorbent materials of palladium reported before. Furthermore, Et-Tol-DAPhen extraction resin could selectively uptake Pd 2+ from a simulated acidic nuclear waste solution containing 20 different kinds of ions with the separation factor SF Pd/M values as high as 100 to 10,000. Moreover, although the adsorption efficiency had a slight decrease after 5 times of adsorption-desorption process, it still remained at a high level. This new extraction resin displayed a potential application prospect in the field of separation and recovery of Pd 2+ from acidic nuclear liquid waste .
研究领域:
化学工程
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Huiling Li,Jingkun Yu,Weibin Wang,Juan Ding,Yongming Sui
Direct formic acid fuel cells (DFAFCs) are considered promising power sources for next-generation portable electronic devices due to their high theoretical energy density, excellent storage stability, and low fuel permeability. However, the multistep nature of the formic acid oxidation (FAO) pathway increases the complexity of designing efficient anode catalysts, posing a significant challenge to the commercialization of DFAFCs. Here, we present a unique example of significantly enhancing the catalytic performance of Pd-based catalysts for FAO through facet effect-regulated nitrogen occupation. Our approach involves the synthesis of nitrogen-doped Pd nanocubes (NCs) and cuboctahedrons (COs). Theoretical and experimental analyses reveal that the subsurface octahedral (O) site N occupation on the (100) facet reduces the energy barrier for the complete FAO process, thereby significantly enhancing the catalytic activity of PdN NCs. In contrast, the tetrahedral (T) site N occupation on the (111) facet increases the adsorption free energy difference between *HCOO and *COOH, which reduces the accumulation of CO and endows PdN COs with superior catalytic stability. This study provides valuable insights for the design of advanced anode catalysts in DFAFCs.
研究领域:
能源材料
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电化学
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催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CATALYSIS LETTERS
·
2021
·Vol. 151
·期 10
·3004-3010
·
IF 3.186
Zhou Junjie,Huang Yu,Shen Jialu,Liu Xiang
The production of H 2 from non-fossil sources is a key research challenge to contributing solving the forthcoming energy problem. Aqueous solutions of tetrahydroxydiboron have very recently appeared as a H 2 source, from which both hydrogen atoms are provided by water, in the presence of highly sophisticated nanocatalysts. Herein, commercial and cheap Pd/C is shown to be an efficient and recyclable catalyst for H 2 evolution upon tetrahydroxydiboron hydrolysis. Graphic Abstract
研究领域:
化学
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2014
·
IF 4.086
Jie-Ning Zheng,Li-Li He,Fang-Yi Chen,Ai-Jun Wang,Meng-Wei Xue,Jiu-Ju Feng
In this work, bimetallic alloyed platinum-palladium (PtPd) nanoflowers are fabricated by one-pot solvothermal co-reduction of Pt (II) acetylacetonate and Pd (II) acetylacetonate in oleylamine system. The as-prepared nanostructures show the enhanced electrocatalytic activity for oxygen reduction reaction (ORR), dominated by a four-electron pathway based on the Koutecky-Levich plots, mainly owing to the inhibition of the formation of Pt–OH ad via the downshift of d-band center for Pt. Meanwhile, PtPd nanoflowers display good methanol tolerance and improved stability for ORR. The chronoamperometry test reveals that the current of PtPd nanoflowers remains 45.9% of its original value within 6000 s, much higher than those of commercial Pt (36.7%) and Pd (32.2%) black catalysts. Therefore, PtPd nanoflowers with unique interconnected structures can be used as a promising cathode catalyst in direct methanol fuel cells.
研究领域:
材料科学
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化学工程
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能源科学
✓ 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
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2022
·Vol. 29
·期 16
·e202203142
·
IF 5.02
Jingwen Luo,Anqi Huang,Yao-Yue Yang,Xing-Yu Ma,Quan-Liang Chen,Junxian Chen,Yajuan Wu
Graphical Put to good use : A Pd-doped Co (Pd/Co) catalyst with high Pd atom utilization efficiency was designed and prepared for hydrogenation of nitroarenes. Its catalytic activity was much better than commercial Pd powder (>150 times) in nitrobenzene hydrogenation reaction. This work might provide a simple and low-cost methodology to design and synthesize highly efficient catalysts. Enhancing catalytic performance as well as reducing catalyst cost are the eternal pursuit for the catalysis community. Herein, a simple and effective palladium-doped cobalt (Pd / Co) catalyst with high Pd atom utilization efficiency was synthesized via galvanic replacement reaction for the selective hydrogenation of nitrobenzene with H 2 at room temperature, delivering >99 % yield of aniline with up to 158 times higher catalytic activity than commercial palladium powder. Detailed characterizations and DFT calculations revealed that Co−Pd interaction leads to a decrease in electron density of Pd and the distance between Pd atoms that results in the enhanced catalytic performance. Further experiments indicated that the Pd / Co catalyst serves as a highly efficient, selective, and recyclable catalyst for a range of nitroarene substrates. This work might provide a green and sustainable methodology to design and synthesize highly active catalysts with high utilization efficiency of the noble metals in fundamental and applied research.
研究领域:
催化化学
·
材料科学
·
理论计算化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Omega
·
2023
·
IF 4.1
Bolin Wang,Yuxue Yue,Yuliang Li,Lu Yu,Hong Tang,Haifeng Zhang,Feng Feng
Imidazolium-based ionic liquid mixtures with [NO3]− and [AlCl4]− anions were used as oxidizing agents for the dissolution of Au, Pd, and Pt metals under mild conditions. The thermodynamic reduction of [NO3]− to [NO] is catalyzed by [AlCl4]− anions and coupled with the oxidation process of noble metals. The developed ionic liquid system for dissolving Au can reactivate the Au0 formed in the deactivation process of the catalyst in vinyl chloride production. This demonstrates the relevance of the here-presented work for technical noble metal recycling.
研究领域:
化学
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材料科学
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nano Research
·
2023
·Vol. 16
·期 7
·9116-9124
·
IF 9.9
Si Lianxi,Li Hui,Zhang Yu,Zhang Donghao,An Xiaowei,Yao Mengmeng,Shao Yuanyuan,Zhu Jesse,Hu Shi
Ultrathin Pd nanosheets (NSs) have great advantages in catalysis due to their large specific surface area and high percentage of under-coordinated atoms. However, the electrochemical performance still can be improved via composition-controllable growth of their solid solution. Herein, seeded alloying strategy was proposed to synthesize Pd-Cu solid solution from Pd NSs and Pd-Cu nanostructures with tunable molar ratios obtained by changing the amount of Cu precursor. As compared to the pristine Pd NSs, the Pd-Cu solid solution shows significantly enhanced methanol oxidation reaction (MOR) performance over those of Pd NSs and homemade Pd/C as the incorporation of Cu weakens the adsorption of CO intermediate on Pd in the MOR process. The choice of template is pivotal to the growth, as a shape-dependent behavior could be identified in the alloying of Cu with Pd nanosheets enclosed by {111} and {100} facets, Pd nanocubes enclosed by {100} facet, and Pd nano-tetrahedrons enclosed by {111} facet. The Pd-Cu solid solution with tunable composition can only be obtained from Pd NSs and the shape-dependent alloying process is mainly determined by the diffusion barrier and the minimum diffusion depth of the different facets.
研究领域:
材料科学
·
电化学
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）