JOURNAL OF HAZARDOUS MATERIALS
·
2018
·
IF 6.434
Zimo Lou,Yizhou Li,Jiasheng Zhou,Kunlun Yang,Yuanli Liu,Shams Ali Baig,Xinhua Xu
Titanium carbide (TiC) with excellent electrical conductivity, chemical and thermal stabilities has been recognized as one of the most promising electrocatalysts. A novel cathode, titanium carbide doped palladium/nickel foam (TiC-Pd/Ni foam), was synthesized via electroless deposition to improve the performance of Pd/Ni foam in electrocatlytic hydrodechlorination (ECH). TiC can be co-precipitated onto the surface of cathode during galvanic replacement reaction between Pd(II) solution and Ni foam. Both constant potential and constant current tests proved that TiC-Pd/Ni foam cathode performed remarkably higher activity for 2,4-dichlorobenzoic acid (2,4-DCBA) than Pd/Ni foam cathode, owing to the excellent conductivity of TiC and enhanced water dissociation over TiC-Pd/Ni foam cathode. Under the optimized reaction conditions of –0.85 V ( vs Ag/AgCl), electrolyte of 10 mM and initial pH of 4, 99.8% of aqueous 2,4-DCBA (0.2 mM) was removed within 90 min. The removal process of the aqueous 2,4-DCBA obeyed first-order decay kinetic model. Over 86.3% of 2,4-DCBA can still be removed by TiC-Pd/Ni foam cathode in the fifth consecutive run within 120 min, which was much higher than that of Pd/Ni foam cathode (37.5%). Consequently, TiC-Pd/Ni foam cathode was a promising design for enhanced ECH activity and reduced operation cost.
研究领域:
环境科学
·
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2016
·
IF 3.014
Xiaomeng Li,Ming Wen,Dandan Wu,Qingsheng Wu,Jiaqi Li
For the exploration of catalysts with excellent performance in alkaline fuel cells, high-performance two-dimensional (2D) Pd-on-NiCu nanosheets were synthesized through the kinetics controlling synthesis of NiCu nanosheets followed by Pd nanoparticles (NPs) embedding treatment at room temperature. In which case, well-dispersed Pd NPs with the average diameter of ∼4 nm are embedded on NiCu nanosheets (BET surface area of 180.7 m 2 g −1 ). Pd-on-NiCu nanosheets exert remarkable high performance in electrocatalytic activity, methanol-tolerance and stability, the electrocatalytic mass activity of Pd-on-NiCu nanosheets is 1827 mAmg −1 , which is over 6-fold higher than that of commercial Pd/C (289 mAmg −1 ), and the current density of the electrocatalyst decreases after 300 cycles of only 6%. Therefore, Pd-on-NiCu nanosheets can be considered as one of the most promising candidates for fuel cells 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
INTERNATIONAL JOURNAL OF ENERGY RESEARCH
·
2019
·Vol. 43
·期 8
·3284-3294
·
IF 3.343
Xiaoyang Wan,Xuefeng Wei,Juan Miao,Ruichang Zhang,Jun Zhang,Qingshan Jason Niu
Summary A wide compositional range of Pd-Ni/Cd on polypyrrole (PPy)-modified Ti plates (Pd-Ni/Cd/PPy/Ti) was fabricated via electrochemical deposition. The hydrogen absorption properties of the prepared Pd-Ni/Cd/PPy/Ti electrodes were evaluated using cyclic voltammetry and chronoamperometry in acidic media. The optimal Pd 36 -Ni 7 /Cd 57 /PPy/Ti electrode achieved a hydrogen storage capacity of 331.3 mC cm −2 mg −1 and an H/Pd ratio of 0.77. The enhancement of the hydrogen storage was attributed to a synergistic effect between the Pd-Ni/Cd catalysts. The surface morphology, crystallinity, and chemical composition of the Pd-Ni/Cd/PPy/Ti electrode were characterized using scanning electron microscope (SEM), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS), respectively. Hydrogen spillover occurred on the trimetallic catalysts, and secondary hydrogen spillover occurred on the PPy/Ti support. The enhanced hydrogen sorption capacity was due to both the synergistic effect of the trimetallic catalysts and the assistance of PPy, making Pd-Ni/Cd/PPy/Ti a promising hydrogen storage material.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Lu Zhang,Guijiu Xie,Fuyi Liu,Huiming Ji
Hydrogen sensors are very important for real-time detection of hydrogen leakage. In this study, a Pd-Ni film hydrogen sensor with high hydrogen response and selectivity was fabricated. A 1.3 µm-thick organosilica membrane was coated on the surface of Pd-Ni alloy film by sol-gel process and hot-coating method to fabricate a 1,2-bis(triethoxysilyl)methane (BTESM)-coated Pd-Ni film hydrogen sensor, which endows the sensor with superior H 2 selectivity due to the molecular sieve property. And the gas sensing performance was tested at optimum operating temperature. The results show higher response is obtained in both N 2 and air atmosphere by hybrid organosilica membrane modification on the Pd-Ni film sensor. Very importantly, the response of the sensor to hydrogen is greatly improved and well maintained in the presence of oxygen, although the response/recovery time increased. The organosilica membrane has high permeability to hydrogen with the kinetic dimater of 0.289 nm while effectively inhibits the permeation of relatively larger gas molecule such as oxygen (0.34 nm) and methanol (0.38 nm), resulting in excellent selectivity to H 2 . The mechanism of response and selectivity enhancement is explored.
研究领域:
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2023
·
IF 4.7
Qiqi Lu,Xiu-Zhi Wei,Haiyong Wang,Qi zhang,Xinghua Zhang,Lungang Chen,Jianguo Liu,Longlong Ma
The selective hydrogenation of nitrile represents an atom-economical and reliable method to synthesize primary amine, a privileged compound in chemistry, biology, and medicine. However, this approach often displays severe selectivity issues, and additives or reducing agents are generally required to solve this problem. In this work, we aim to synthesize primary amine on a green catalytic system and probe into the catalytic mechanism of Pd-Ni interaction using benzonitrile (BN) as a model compound. The nitrile hydrogenation reaction was catalyzed by bimetallic Pd-Ni oxide nanospecies confined in Silicalite‑1 (S-1) zeolite using H 2 as hydrogen donor without any additive which was environmentally friendly and economic. A 92% yield of benzylamine (BA) was achieved on the [email protected] catalyst with a turnover number (TON) of 1667, and such BA yield was still maintained in upscaling experiment. Detailed characterizations shed light on the mechanism of the extraordinary performance of Pd-Ni oxide nanospecies on base-free nitrile hydrogenation.
研究领域:
化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2018
·Vol. 8
·期 7
·1858-1866
·
IF 5.365
Qingjie Meng,Jiajia Liu,Xiaole Weng,Pengfei Sun,Jawwad A. Darr,Zhongbiao Wu
Noble metals, e.g. Pd, are often made into hybrid or composite catalysts (with less expensive materials) to oxidize industry-source emitted volatile organic compounds (VOCs) at low temperatures. In general, the loadings of these metals should be optimized to reduce costs whilst maintaining activity. There exists the possibility to obtain highly active catalysts with low loadings of noble metals by properly tuning the valence state of the metal(s). However, the relationship between the valence state and its effect on catalyst performance is still a matter of debate. In this article, we used supercritical water (sc-H2O), in the presence of oxidizing or reducing gases, as a feasible reaction medium to synthesize Pd/NiO hybrid nano-catalysts and in situ modify the valence state of Pd. After subjecting the catalysts to a range of analytical techniques, including XRD, H2-TPR, DRIFT, TPSR, etc., we unveiled that Pd0 is more active than PdOx and metal oxides in the catalytic oxidation of toluene. This is mainly because the stabilized Pd0 is capable of activating gaseous oxygen (and toluene) at low temperatures and returning to the original state by toluene even with excess oxygen. Although PdOx could desorb active oxygen under a reducing atmosphere and might assist in the oxygen spillover from NiO, it is difficult to convert into Pd0 in an oxygen-rich environment. The developed Pd0-dominated catalyst was found to be robust and highly active after an ageing test with and without water vapour.
研究领域:
催化化学
·
环境科学
✓ 已验证
DOI
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2021
·Vol. 27
·期 58
·14472-14477
·
IF 5.236
Hongjing Wang,Shiqian Jiao,Songliang Liu,Hugang Zhang,You Xu,Xiaonian Li,Ziqiang Wang,Liang Wang
Graphical The mesoporous PdNi/Ni nanoparticles assembled nanotubes (mPdNi/Ni NTs) have been synthesized via replacement reaction, in which nickel nanowires serve as sacrificial template to form tubular structure and the diblock copolymer induce the formation of mesoporous structures. Due to the mesoporous nanoparticle structure and tubular geometry, the mPdNi/Ni NTs have better catalytic performance than mesoporous Pd nanotubes and commercial Pd black for ethanol oxidation reaction. The optimization of structure and composition is essential to improve the performance of catalysts. Herein, mesoporous nanoparticles assembled PdNi/Ni nanotubes (mPdNi/Ni NTs) are successfully fabricated using nickel nanowires as sacrificial template. The combination of nanotubular structure with mesoporous nanoparticle morphology can provide facilitated transfer channels and sufficient active sites, allowing the full contact and reaction between catalysts and reactants. Therefore, the synthesized mPdNi/Ni NTs exhibite superior ethanol oxidation performance to mesoporous Pd nanotubes and commercial Pd black. This study proposes a rational strategy for the development of nanoparticle assembled nanotubes with surface mesoporous morphology, which can greatly improve catalytic performance in various electrocatalytic fields.
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
Catalysts
·
2023
·Vol. 14
·期 1
·24
·
IF 3.9
Chunlian Luo,Luwei Chen,Abdullah N. Alodhayb,Jianhua Wu,Mingwu Tan,Yanling Yang
The development of catalysts for low-temperature methane combustion is crucial in addressing the greenhouse effect. An effective industrial catalyst strategy involves optimizing noble metal utilization and boosting metal–metal interaction. Here, the PdNi-H catalyst was synthesized using the self-assembly method, achieving the high dispersion and close proximity of Pd and Ni atoms compared to the counterparts prepared by the impregnation method, as confirmed by EDS mapping. The XRD and TEM results revealed Pd2+and Ni2+doping within the CeO2lattice, causing distortions and forming Pd-O-Ce or Ni-O-Ce structures. These structures promoted oxygen vacancy formation in CeO2, and this was further confirmed by the Raman and XPS results. Consequently, the PdNi-H catalyst demonstrated an excellent redox ability and catalytic activity, achieving lower ignition and complete methane burning temperatures at 282 and 387 °C, respectively. The highly dispersed PdNi species played a pivotal role in activating methane for enhanced redox ability. Additionally, the narrow size distribution range contributed to more vacancies on the surface of CeO2, as confirmed by the XPS results, thereby facilitating the activation of gas phase oxygen to form oxygen species (O2−). This collaborative catalytic approach presents a promising strategy for developing efficient and stable methane combustion catalysts at low temperatures.
研究领域:
催化化学
·
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Jun Zhang,Xinlan Xu,Lanyu Luo,Tiantian Peng,Boyu Liu,Lingying Jiang,Meng Jin,Rong Wang,Huan Yi,Weimin Wu,Shi-Yu Lu
The selective exposure of active surfaces has garnered exceptionally widespread attention in enhancing electrocatalytic performance for oxygen reduction reactions (ORR). Nevertheless, because unmanageable growth thermodynamics and kinetics, the exposure of active surface not only hinders the formation of high-index facets but also induces irreversible reconstruction of low-index facets at high-potential region. Therefore, the controlled synthesis of Pd-based nanocrystals featuring high/low-index facets is highly desirable. In this study, bimetallic PdNi alloys with high/low-index facets were successfully synthesized through crystal structure engineering. Assisted by Ni 2+ , the transition from low-index facets to high-index facets was achieved. These structural features endow PdNi alloy nanocrystals with highest half-wave potential (0.893 V), mass activity (0.127 A mg −1 ), and specific activity (0.926 mA cm −2 ) in ORR. Additionally, this alloy nanocrystals follow an efficient four-electron reduction pathway and exhibit excellent long-term stability over 10,000 cycles. Density functional theory calculations suggest that the outstanding ORR performance stems from the minimal downhill energy gradient in the rate-determining step, and the reduced oxygen adsorption energy on the PdNi alloy (311) crystal plane. This innovative strategy adds more potentialities for development and commercial application in fuel cells.
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
Nano Research
·
2014
·Vol. 7
·期 9
·1337-1343
·
IF 6.963
Xiang Ji,Li Peng,Chong Hanbao,Feng Li,Fu Fangyu,Wang Zhuang,Zhang Shilin,Zhu Manzhou
A simple and efficient solution-based method for the synthesis of Pd-Ni bimetallic nanoparticles (NPs) has been developed. A series of Pd-Ni bimetallic NPs were readily achieved by reduction of PdCl 2 and Ni(acac) 2 (acac = acetylacetonate) in the presence of oleylamine (OAm), oleic acid (OA) and benzyl alcohol. Furthermore, by using high-resolution transmission electron microscopy (HRTEM), energy-dispersive spectrometry (EDS) mapping and X-ray diffraction (XRD), we demonstrate that the as-prepared Pd-Ni bimetallic NPs have core-shell structures with a Pd-rich core and a Ni-rich shell. In addition, the as-obtained Pd-Ni bimetallic NPs with varying compositions show excellent catalytic activities in the Miyaura-Suzuki reaction. When the nickel molar percentage was 0.23 to 0.65, the conversion with the as-obtained Pd-Ni bimetallic catalysts was above 90%. It is believed that this strategy can be employed to produce a variety of other well-defined core-shell type multimetallic nanostructures.
研究领域:
材料科学
·
化学
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2017
·
IF 3.582
Yuanxin Du,Kun Wang,Qingxi Zhai,Akang Chen,Zhiwei Xi,Jian Yan,Xi Kang,Man Chen,Xiaoyou Yuan,Manzhou Zhu
Hydrolysis reaction of ammonia borane (AB) has been considered as a safe and efficient hydrogen generation method, in which designing cost-effective and high-performance catalysts plays vital role. In this work, we have developed well dispersed palladium-nickel hollow nanospheres (PdNi HNSs) with tunable shell thickness and compositions via a facile galvanic replacement approach. The as-prepared PdNi HNSs show composition-dependent catalysis in the hydrolytic dehydrogenation of AB. The Pd 84 Ni 16 /C exhibiting sphere-shaped hollow interiors with average 70 nm particle size and 10 nm thin wall, presents the highest catalytic activity with the turnover frequency of 76.0 (mol H 2 min −1 (mol Pd) −1 ) and the activation energy of 33.5 kJ mol −1 . The superior catalytic effect of PdNi HNSs in enhancing hydrolysis efficiency of AB can be ascribed to two major factors: (1) high active surface areas of the unique hollow structure; (2) enhanced H adsorption attributed to the coupling between Pd and Ni induces polarization charges on Pd catalytic sites, which is indicated by the first-principles calculation and X-ray photoelectron spectroscopy studies. Furthermore, the catalysts exert good long-term recycling stability and catalytic activity for the hydrolytic dehydrogenation of AB. This work represents a strategy may hopefully be extended to synthesize other Pd-based hollow nanostructure with reduced Pd usage and increased catalytic active sites, and also sheds light on the exploration of utilizing interatomic interactions to regulate species adsorption/activation for highly efficient catalytic performance.
研究领域:
材料科学
·
催化化学
·
能源化学
✓ 已验证
DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2022
·
IF 10.753
Xiao-Qiu Lin,Jia-Mei You,Ling-Yu Meng,Naoko Yoshida,Jing-Long Han,Cong-Ju Li,Ai-Jie Wang,Zhi-Ling Li
Tetrabromobisphenol A (TBBPA), a hazardous and persistent flame retardant , has been widely detected in the natural aquatic system. The acceleration of reductive debromination (rate-limiting process) is vital during the decomposition and detoxification of TBBPA. This study achieved superior TBBPA electrochemical reductive debromination performance by nano Pd doped Ni foam electrode (4.8 times higher than Ni foam electrode). The optimal TBBPA reductive debromination performance was obtained under −1.2 V of cathode potential, 1.2 wt% of Pd loading, 10 mg L −1 of TBBPA and 100 mM of Na 2 SO 4 as the electrolyte solution. UPLC-QTOF-MS verified that Br atoms in TBBPA were removed sequentially to form bisphenol A as the major product. Most TBBPA was reductively debrominated by atomic H* through indirect hydrodebromination, evidenced by the atomic H* quenching test. The higher solution conductivity and appropriate TBBPA concentration would contribute to the debromination efficiency. Excessive H 2 generation whether by over negative potential or H atom richness electrolyte largely disturbed the reaction process and restricted the debromination. The improved generation of reductant (H*) ads Pd was the most significant, while excessive Pd loading would make aggregation and limit the debromination efficiency. The study confirmed the optimization strategies of conditions for Pd/Ni foam electrode and revealed the related function mechanism for stimulating TBBPA electrochemical reduction, giving suggestions for the efficient removal of TBBPA in the aquatic environment.
研究领域:
环境科学
·
电化学
·
污染控制
✓ 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）