DALTON TRANSACTIONS
·
2015
·Vol. 44
·期 31
·13906-13913
·
IF 4.197
Kunpeng Song,Peng Liu,Jingyu Wang,Lei Pang,Jian Chen,Irshad Hussain,Bien Tan,Tao Li
Novel dual-porous carbon-supported palladium nanoparticle (Pd NP) catalysts were prepared by sequential carbonization and reduction of microporous organic polymer-encaged PdCl2. The diverse pore structure of microporous organic polymers provides a reservoir for the palladium precursors and prevents Pd NPs from sintering during the carbonization and reaction. The microporous structure has a significant effect on the size and dispersion of palladium NPs. The average size of the Pd NPs (in the range of 4–6 nm) was tuned by changing the pore size distribution and the carbonization temperature. The resulting carbon-supported Pd NPs were characterized by TEM, BET, XRD, and XPS and the Pd loading was calculated by AAS. The encaged Pd NP catalysts prepared by this methodology exhibited outstanding stability and reusability in the Heck reaction and could be reused at least 10 times without appreciable loss of activity.
研究领域:
材料化学
·
纳米催化
·
有机合成方法学
·
多孔材料
·
绿色化学
✓ 已验证
DOI
高影响因子
MICROCHIMICA ACTA
·
2016
·Vol. 183
·期 8
·2403-2409
·
IF 4.831
Ye Cui,Zhong Xia,Wang Min-Qiang,Chai Yaqin,Yuan Ruo
A glassy carbon electrode (GCE) was modified with a nanocomposite consisting of tetraoctylammonium bromide (TOAB), C 60 fullerene, and palladium nanorods (PdNRs). The PdNRs were hydrothermally prepared and had a typical width of 20 ± 2 nm. The nanocomposite forms stable films on the GCE and exhibits a reversible redox pair for the C 60 /C 60
− system while rendering the surface to be positively charged. The modified GCE was applied to fabricate an electrochemical biosensor for detecting acetylcholinesterase (AChE) by measurement of the amount of thiocholine formed from acetylthiocholine, best at a working voltage of −0.19 V (vs. SCE). The detection scheme is based on (a) measurement of the activity of ethyl paraoxon-inhibited AChE, and (b) measurement of AChE activity after reactivation with pralidoxime (2-PAM). Compared to the conventional methods using acetylthiocholine as a substrate, the dual method presented here provides data on the AChE activity after inhibition and subsequent reactivation, thereby yielding credible data on reactivated enzyme activity. The linear analytical range for AChE activity extends from 2.5 U L −1 to 250 kU·L −1 , and the detection limit is 0.83 U L −1 .
Cyclovoltammetric acetylcholinesterase (AChE) activity assay is constructed based on the palladium nanorods composited with functionalized C 60 fullerene (PdNR/C 60 + TOAB), which aims to measure the signal change between ethyl paraoxon-inhibited and subsequent pralidoxime (2-PAM)-reactivated AChE activity.
研究领域:
生物传感
·
酶学分析
·
纳米材料修饰电极
·
电化学检测
·
毒理学
✓ 已验证
DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2016
·Vol. 164
·期 2
·B48
·
IF 3.014
Yu Zhang,Zhi Xia,Qianzhu Li,Guofeng Gui,Gaoyu Zhao,Longli Lin
A novel acetylcholinesterase (AChE) biosensor for the detection of chlorpyrifos has been developed based on the immobilization of AChE on palladium-reduced graphene nanocomposites (rGO@Pd) modified glassy carbon electrode (GCE). The nanocomposites were synthesized by a one-step electrochemical co-deposition approach. Pd nanoparticles and rGO can be alternately attached onto the electrode surface, forming an interpenetrating network, which with excellent conductivity, catalysis, and biocompatibility offered an extremely hydrophilic surface for AChE adhesion. Under optimum conditions, the biosensor detects chlorpyrifos in two linear ranges, one is from 0.71 to 5.70 μM and the other is from 14.26 to 71.13 μM. The detection limit is 0.23 μM and the biosensor exhibits good performance such as reproducibility and stability, which makes it possible to provide a new and promising tool for the analysis of enzyme inhibitors.
研究领域:
环境科学
·
生物传感技术
·
农药检测
✓ 已验证
DOI
高影响因子
BIOSENSORS & BIOELECTRONICS
·
2019
·
IF 9.518
Jinglong Fang,Guanhui Zhao,Xue Dong,Xuan Li,Juncong Miao,Qin Wei,Wei Cao
An electrochemiluminescence (ECL) analytical platform was proposed for ultrasensitive detection of amyloid-β proteins (Aβ) based on the ECL resonance energy transfer (ECL-RET). In this work, gold nanoparticles-functionalized graphitic carbon nitride nanosheets (g-C 3 N 4 @Au NPs) and palladium nanoparticles-coated Metal organic framework (Pd NPs@NH 2 -MIL-53) were synthesized, which were as ECL donor and ECL acceptor respectively. A strong cathode ECL emission was obtained from the g-C 3 N 4 @Au NPs when used K 2 S 2 O 8 as its co-reactant. Here, Au NPs not only was used as an accelerator to enhance and stabilize the ECL signal, but also a connector for attaching Aβ antibody. In addition, NH 2 -MIL-53(Al) was selected as a label material for supporting Pd NPs to synergistically increase the intensity and range of UV-visible absorption. The ECL signal of g-C 3 N 4 @Au NPs was intensely decreased when the ECL acceptor probe Pd NPs@NH 2 -MIL-53 was incubated onto the modified GCE by way of the specific recognition. Under the optimal condition, a wide detection range from 10 fg/mL to 50 ng/mL and a low detection limit of 3.4 fg/mL (S/N = 3) were obtained. In consideration of favorable specificity, stability and reproducibility, the proposed method was successfully applied for Aβ detection in actual human serum samples and could be a potential analytical tool for sensitive molecular trace detection in clinical analysis.
研究领域:
分析化学
·
生物医学工程
·
临床诊断
✓ 已验证
DOI
高影响因子
RSC Advances
·
2017
·Vol. 7
·期 64
·40462-40469
·
IF 3.108
Yingxia Wang,Zhong Xiong,Yanzhi Xia
In this work, novel branched palladium–gold (PdAu) bimetallic nanowires supported on graphene (PdAu/graphene) were fabricated at relatively low temperatures for the first time by a one-pot co-reduction method with the aid of poly(diallyldimethyl-ammonium chloride). The structural characteristics of PdAu/graphene were confirmed by X-ray diffraction, X-ray photoelectron spectroscopy, transmission electron microscopy, energy-dispersive X-ray spectroscopy, high-angle annular dark-field scanning transmission electron microscopy and element mapping observations. The electrochemical properties of the PdAu/graphene were characterised by cyclic voltammetry and chronoamperometry (CA) in the formic acid oxidation reaction. Compared with a commercial Pd/C catalyst, the PdAu/graphene catalyst prepared in this work exhibited enhanced electrocatalytic activity including a higher oxidation current density, enhanced CO tolerance, and a more negative onset potential. Moreover, CA analyses demonstrated that PdAu/graphene shows higher stability than the Pd/C catalyst. The PdAu/graphene catalyst exhibited higher activity and strong poisoning resistance, which could be attributed to its special branched structure from PdAu nanowires.
研究领域:
纳米催化
·
电化学
·
材料科学
·
能源化学
·
表面科学
·
电分析化学
✓ 已验证
DOI
高影响因子
CHINESE JOURNAL OF CHEMISTRY
·
2013
·Vol. 31
·期 3
·371-376
·
IF 0.917
Wei Zhu,Haoyang Wang,Haihui Peng,Guosheng Liu,Yinlong Guo
Pd-catalyzed oxidative coupling reaction was of great importance in the aromatic C H activation and the formation of new C O and C C bonds. Sanford has pioneered practical, directed C H activation reactions employing Pd(OAc) 2 as catalyst since 2004. However, until now, the speculated reactive Pd(IV) transient intermediates in these reactions have not been isolated or directly detected from reaction solution. Electrospray ionization tandem mass spectrometry (ESI-MS/MS) was used to intercept and characterize the reactive Pd(IV) transient intermediates in the solutions of Pd(OAc) 2 -catalyzed oxidative coupling reactions. In this study, the Pd(IV) transient intermediates were detected from the solution of Pd(OAc) 2 -catalyzed oxidative coupling reactions by ESI-MS and the MS/MS of the intercepted Pd(IV) transient intermediate in reaction system was the same with the synthesized authentic Pd(IV) complex. Our ESI-MS(/MS) studies confirmed the presence of Pd(IV) reaction transient intermediates. Most interestingly, the MS/MS of Pd(IV) transient intermediates showed the reductive elimination reactivity to Pd(II) complexes with new C O bond formation into product in gas phase, which was consistent with the proposed reactivity of the Pd(IV) transient intermediates in solution.
研究领域:
有机化学
·
金属有机化学
·
分析化学
·
催化化学
·
质谱学
✓ 已验证
DOI
高影响因子
Journal of Physical Chemistry C
·
2014
·
IF 4.835
Fang Niu,Shuiqing Li,Yichen Zong,Qiang Yao
A controlled one-step synthesis of titania-supported palladium (Pd/TiO2) nanoparticles is demonstrated by using a premixed stagnation swirl flame with an ultrafine spray feeding system. The new method produces well-dispersed palladium clusters on the surface of TiO2 particle. The low-temperature methane catalytic oxidation indicates that the flame-made Pd/TiO2 possesses activity apparently higher than that of the impregnated one under the same Pd loading. For the first time, we observe a special pinched hysteresis loop of catalytic activity of Pd/TiO2 nanoparticles from the curves of CH4 conversion versus temperature during heating–cooling cycles. Thermal stability analysis confirms the complex coexistence and transformation of metallic Pd and PdO in Pd/TiO2 particles. Further morphological characterization reveals the oxidation rate is controlled by the metallic Pd content on the particle surface, whereas the deactivation of the catalysts is mainly due to the Pd dispersion decrement. The competition between the Pd dispersion decrement and the PdO reduction at the surface may result in the pinched hysteresis loop of Pd/TiO2 catalysts during low-temperature methane combustion.
研究领域:
催化化学
·
纳米材料科学
·
环境催化
·
能源化学
·
表面科学
✓ 已验证
DOI
高影响因子
Catalysts
·
2019
·Vol. 9
·期 5
·410
·
IF 3.444
Lei Ma,Shiyan Yuan,Taotao Jiang,Xiangming Zhu,Chunshan Lu,Xiaonian Li
Sulfur species (e.g., H2S or SO2) are the natural enemies of most metal catalysts, especially palladium catalysts. The previously reported methods of improving sulfur-tolerance were to effectively defer the deactivation of palladium catalysts, but could not prevent PdO and carrier interaction between sulfur species. In this report, novel sulfur-tolerant SiO2supported Pd4S catalysts (5 wt. % Pd loading) were prepared by H2S–H2aqueous bubble method and applied to catalytic complete oxidation of methane. The catalysts were characterization by X-ray diffraction, Transmission electron microscopy, X-ray photoelectron Spectroscopy, temperature-programmed oxidation, and temperature-programmed desorption techniques under identical conditions. The structural characterization revealed that Pd4S and metallic Pd0were found on the surface of freshly prepared catalysts. However, Pd4S remained stable while most of metallic Pd0was converted to PdO during the oxidation reaction. When coexisting with PdO, Pd4S not only protected PdO from sulfur poisoning, but also determined the catalytic activity. Moreover, the content of Pd4S could be adjusted by changing H2S concentration of H2S–H2mixture. When H2S concentration was 7 %, the Pd4S/SiO2catalyst was effective in converting 96% of methane at the 400 °C and also exhibited long-term stability in the presence of 200 ppm H2S. A Pd4S/SiO2catalyst that possesses excellent sulfur-tolerance, oxidation stability, and catalytic activity has been developed for catalytic complete oxidation of methane.
研究领域:
催化化学
·
环境催化
·
材料化学
·
能源化学
·
表面科学
✓ 已验证
DOI
高影响因子
CATALYSIS LETTERS
·
2024
·Vol. 154
·期 7
·3858-3866
·
IF 2.3
Lin Baining,Du Xuhong,Huang Zhijing,Liu Gonggang,Zhou Yonghua,Xiao Zhihong,Tu Yusong
Reducing the ignition temperature of aromatic volatile organic compounds (VOCs) is a long-term pursuit for environmental pollution treatment and industrial application. In this paper, the toluene catalytic combustion was ignited at ultra-low temperature of 73 °C over a poplar wood monolithic catalyst with highly dispersed Pd particles coated by nano-thick graphited carbon layer via in-situ carbonization. Combing the characterizations and DFT calculations, the satisfying catalytic performance could be attributed to two aspects: (i) the unrestricted mass transfer of reactant and the high dispersity of Pd were simultaneously ensured in the straight micrometer-channel with abundant surface anchoring groups of poplar wood; (ii) the nano-thick graphited carbon layer on Pd significantly enhanced the oxygen activation. Given the low cost of economic wood and facile preparation technique, this work opened up new alternative for the preparation of highly dispersed noble metal catalyst and the low temperature catalytic combustion of aromatic VOCs in industry. Graphical
研究领域:
环境污染治理
·
催化化学
·
材料科学
·
工业应用
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
·
2014
·Vol. 2
·期 19
·6740-6746
·
IF 0
Weining Sun,Xiaofeng Lu,Yan Tong,Junyu Lei,Guangdi Nie,Ce Wang
In this report, a palladium/polypyrrole/polyacrylonitrile (Pd/PPy/PAN) composite nanofiber membranes was synthesized by a one-pot redox polymerization process between pyrrole monomers and Na2PdCl4 in the presence of electrospun PAN nanofibers, without the introduction of any other surfactants or reductants. The as-prepared Pd/PPy/PAN nanofiber membrane exhibited good catalytic performance towards hydrogen generation from the hydrolysis of ammonia borane (AB). The apparent activation energy (Ea) was calculated to be about 33.5 kJ mol−1. In addition, the Pd nanoparticles (Pd NPs) were encapsulated in PPy layers on the surface of the PAN nanofibers, enabling the catalyst to be stable against poisoning and easily separated from the suspension system. The catalytic activity does not weaken after five cycles. This study indicated that the obtained Pd/PPy/PAN composite nanofiber membrane could be applied as an alternative in exploring new catalysts for hydrogen generation, as hydrogen is an important fuel as a clean power source.
研究领域:
材料化学
·
纳米催化
·
能源材料
·
高分子科学
·
氢能源
✓ 已验证
DOI
GREEN CHEMISTRY
·
2019
·Vol. 21
·期 19
·5336-5344
·
IF 9.405
Da Yang,Huan Liu,Lei Liu,Wen-Di Guo,Yong Lu,Ye Liu
An amphiphilic tri-functional ligand (L1) containing a Lewis acidic phosphonium cation, a phosphino-fragment and a hydrophilic sulfonate anion (–SO3−) enabled Pd(OAc)2 to efficiently co-catalyze the hydroxycarbonylation of terminal alkynes towards α,β-unsaturated carboxylic acids. These incorporated functional groups synergistically promoted the reaction, which proved more effective than the ligands lacking –SO3− and/or phosphonium and the mechanical mixtures of the individual functional groups independently. The molecular structure of Pd-L1 indicated that –SO3− in L1 served as a secondary O-donor ligand with reversible coordinating ability, cooperating with the phosphino-fragment to stabilize the Pd-catalyst. The in situ FT-IR analysis verified that the formation and stability of Pd–H active species in charge of hydroxycarbonylation were dramatically facilitated by the presence of L1. It was believed that, over the L1-based Pd-catalyst, H2O was cooperatively activated by the Lewis acidic phosphonium via “acid–base pair” interaction (H2O → P(V)+) and by the hydrophilic SO3−via hydrogen bonding (SO3−⋯H2O), giving rise to the formation of dimeric and mono-nuclear Pd–H species driven by reversible SO3−-coordination. In addition, the L1-based Pd-catalyst could be immobilized in the ionic liquid [Bmim]NTf2 for six-run recycling uses without obvious activity loss and detectable metal leaching.
研究领域:
有机化学
·
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2020
·
IF 5.006
Caoping Yang,Kaijie Li,Junyou Wang,Shenghu Zhou
Pd nanoparticles (NPs) encaged hollow mesoporous silica nanoreactors (Pd@HMSNs) are prepared for hydrogenations of phenol, cresols and chlorophenols to cyclohexanone derivatives. Pd@HMSNs feature ∼ 4 nm Pd NPs in ∼ 16 nm hollow cavities of ∼ 30 nm HMSNs. Such Pd@HMSNs are highly thermally and catalytically stable. At mild reaction conditions, Pd@HMSNs efficiently catalyze hydrogenations of phenol and m -cresol to cyclohexanone derivatives with ≥ 98.3 % selectivity at ≥ 99.0 % conversions. Hydrogenations of o - and m -chlorophenol over Pd@HMSNs give cyclohexanone with ≥ 97.3 % selectivity at 100.0 % conversions, demonstrating a beneficial effect of such HMSNs for consecutive reactions. The confinement of Pd NPs inside hollow cavities of mesoporous nanoreactors greatly promotes collision times of reactant molecules with Pd NPs, resulting in an enhanced catalytic efficiency, while the residence of Pd NPs inside cavities provides a protecting effect for Pd NPs and is beneficial to thermal and catalytic stabilities.
研究领域:
催化
·
纳米技术
·
化学工程
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）