International Journal of Electrochemical Science
·
2023
·
IF 1.5
Min Zhang,Dongmei Fu
A gas-liquid interface approach was developed for the synthesis of ternary Pd-Au-P composites, which were supported on poly(diallyldimethylammonium chloride)-functionalized reduced graphene oxide (PDDA/RGO). The as-synthesized composites were characterized by transmission electron microscopy (TEM), energy dispersive X-ray spectroscopy (EDX), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). The Pd-Au-P-PDDA/RGO composites as an electrochemical dopamine (DA) sensor showed superior electrocatalytic activity and stability toward DA oxidation as compared with Pd- Au-PDDA/RGO and Pd-Au-P/RGO. The enhanced electrochemical performance could be attributed to the effect of electronic structure and long-range disorder and short-range structure due to the doping of P element. By studying the kinetics of DA oxidation, electrochemical DA oxidation was proven to be irreversible and follow Laviron Equation. Using differential pulse voltammetry (DPV), the Pd-Au- P/PDDA/RGO sensor had low detection limit of 0.7 ^M, wide linear range of 3.5-125 ^M and relatively high sensitivity (0.2858 μA/μM), which was suitable for the detection of biological and environmental samples.
研究领域:
生物医学工程
·
材料科学
·
分析化学
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DOI
高影响因子
ChemistryOpen
·
2022
·Vol. 11
·期 4
·e202100301
·
IF 2.63
Yin-Qing Yao,Kai-Chun Zhao,Yi-Ying Zhuang,Xiao-Chao Chen,Yong Lu,Ye Liu
Graphical The one-pot synthesis of 2,5-furandicarboxylic acid from 2-furoic acid was achieved for the first time using a Pd-catalyzed bromination-hydroxycarbonylation tandem reaction in HOAc-NaOAc buffer. The synthesis process provides major improvements compared to previously reported methods, namely using biomass-based 2-furoic acid as low-cost raw material, one-pot synthesis without isolation of intermediate product, and no need for an acidification procedure. The one-pot synthesis of 2,5-furandicarboxylic acid from 2-furoic acid with a yield of 57 % was achieved for the first time using a Pd-catalyzed bromination-hydroxycarbonylation tandem reaction in HOAc-NaOAc buffer. This synthetic protocol shows major improvements compared to previously reported methods, such as using biomass-based 2-furoic acid as low-cost raw material, one-pot synthesis without isolation of intermediate products, and no need for an acidification procedure. Experiments indicate that the involved Xantphos-modified Pd-catalyst and the buffer solution play significant promoting roles for each individual reaction whereas Br 2 (as the brominating reagent) had a negative effect on the second hydroxycarbonylation step, while CO was deleterious for the first bromination step. Hence, in this practical one-pot synthesis, Br 2 should be consumed in the first bromination step as fully as possible, and CO is introduced after the first bromination step has been completed.
研究领域:
有机化学
·
生物质化学
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DOI
PubMed
高影响因子
Catalysis Science & Technology
·
2019
·Vol. 10
·期 1
·138-146
·
IF 5.726
Ting Wang,Xueqin Tao,Yi Xiao,Ganhua Qiu,Yun Yang,Benxia Li
While heterogeneous photocatalysis is regarded as a sustainable strategy to achieve organic reactions for the production of high-value-added organics, photocatalytic efficiency is generally limited by poor charge separation, dull surface catalytic activity and the consequently caused insufficient generation of active species. Herein, the hybrid structures of metal–organic frameworks (MOFs) incorporated with Pd ultrasmall nanocrystals are synthesized, and their photocatalytic performance is evaluated by the oxidative coupling of benzylamine as a model reaction. The photocatalytic activity of the Pd/MIL-125-NH2 hybrid material with an optimal Pd loading is greatly superior to that of the pristine MIL-125-NH2, achieving a high benzylamine conversion rate of 3136 μmol h−1 gcat−1 at 94.08% conversion. The enhanced charge transfer and separation in Pd/MIL-125-NH2 are verified by photoluminescence spectroscopy and photoelectrochemical experiments. Photogenerated reactive oxygen species are probed by 3,3′,5,5′-tetramethylbenzidine (TMB) as an indicator and the reactive intermediates in the photocatalytic systems are identified by in situ ESR detection. The results confirm that the optimized Pd/MIL-125-NH2 hybrid catalyst possesses higher ability for molecule activation and that both superoxide radical (˙O2−) and singlet oxygen (1O2) are the dominant oxidative species in the present photocatalytic system. Therefore, the dual advantages of Pd/MIL-125-NH2 hybrid structures for promoting the photogenerated charge transfer/separation and providing highly catalytic sites for molecule activation contribute to higher photocatalytic activity.
研究领域:
材料科学
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化学工程
·
环境科学
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DOI
高影响因子
ELECTROCHEMISTRY COMMUNICATIONS
·
2015
·
IF 4.847
Tao Yang,Yanxia Ma,Qingli Huang,Guojian Cao,Sheng Wan,Na Li,Hong Zhao,Xia Sun,Fujun Yin
In this work, palladium–iridium nanowires with a Pd/Ir atomic ratio of 2/1 are synthesized through a facile hydrothermal method . Transmission electron microscopy images show that the palladium–iridium nanowires have a uniform diameter below 2 nm and a rough surface with many atomic steps. The electro-catalytic performance of the carbon supported palladium–iridium catalyst towards oxygen reduction reaction has been examined in 0.1 M HClO 4 solution. The carbon supported palladium–iridium catalyst displays comparable catalytic activity but much higher durability in comparison with those of the commercial carbon supported platinum catalyst. The excellent electro-catalysis might be attributed to the high accessible area, rough surface and iridium introduction. The work demonstrates that palladium–iridium nanocrystals are promising electro-catalysts for oxygen reduction electro-catalysis in acid media.
研究领域:
材料科学
·
电化学
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DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2017
·
IF 4.339
Miaomiao Liu,Weiqiang Tang,Yisheng Xu,Hongbo Yu,Hongfeng Yin,Shuangliang Zhao,Shenghu Zhou
Pd-SnO 2 heteroaggregate nanocatalysts were synthesized by in-situ transformation of PdSn bimetallic nanoparticles on alumina. The PdSn bimetallic nanoparticles were prepared by co-reduction of Pd and Sn precursors. The obtained PdSn nanoparticles possibly have a core-shell like structure with Pd cores and Sn-rich shells due to the fast reduction of Pd precursors. The Pd-SnO 2 /Al 2 O 3 heteroaggreagte nanocatalysts were synthesized by calcination of PdSn/Al 2 O 3 in air followed by H 2 reduction. Various characterization techniques, such as HRTEM, XRD and XPS, were used to characterize the PdSn and Pd-SnO 2 . The Pd 3 -(SnO 2 ) 1 /Al 2 O 3 heteroaggreagte nanocatalysts with a ratio of Pd/Sn of 3/1 illustrated enhanced catalytic performances for p -nitroacetophenone and p -nitrobenzaldehyde hydrogenations relative to monometallic Pd nanocatalysts. Theoretical calculations using density functional theory suggested that Pd-SnO 2 facilitates the adsorption of reactants in a higher degree than that of products, thus enhancing the catalytic activity even with partial coverage of Pd surfaces with SnO 2 . The blockage effect of SnO 2 on Pd surfaces is speculated to enhance the catalytic selectivity for p -nitroacetophenone and p -nitrobenzaldehyde hydrogenations over Pd-SnO 2 heteroaggregate nanocatalysts.
研究领域:
催化化学
·
材料科学
·
理论计算
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DOI
高影响因子
Applied Catalysis O: Open
·
2024
·
IF 0
Si Xiong,Aiping Wang,Baohe Wang,Jing Ma,Zhaobang Zhang,Jing Zhu
The complexation of palladium with bidentate phosphine ligand has significant effects on the activity of the catalyst for methoxycarbonylation of ethene. Herein, the influence of the ratio of components, kind and sequence of additives, complexation temperature and time on the catalytic performance were studied, then probable mechanism was proposed, and further kinetic studies were carried out under the optimized conditions. Compared to add Methanesulfonic acid (MSA) after complexation, the addition of an appropriate dose of MSA before complexation rather than after complexation could effectively improve the activity of the catalyst, while the addition of Methyl Propionate (MeP) would reduce the activity of the catalyst. It was worth noting that the weak absorption of [Pd-H] + in 1943 cm −1 was captured in the complex by in situ FT-IR.
研究领域:
催化化学
·
有机化学
✓ 已验证
DOI
SENSORS AND ACTUATORS B-CHEMICAL
·
2016
·
IF 4.758
Li Liu,Yueyuan Li,Lihui Tian,Qin Wei,Wei Cao
A novel and ultrasensitive sandwich-type electrochemical immunosensor was designed for quantitative detection of prostate specific antigen (PSA). The Ag overgrowth in Pd nano-octahedrons, developed Pd-Ag heterodimers (Pd-Ag HDs), loaded on amino functionalized multiwalled carbon nanotubes (MWCNTs-NH 2 ) were employed as labels of secondary antibodies (Ab 2 ). The synergistic effect of Pd-Ag HDs exhibited high electrocatalytic activity towards the reduction of H 2 O 2 . MWCNTs-NH 2 with good dispersion , plentiful amino groups and large specific surface area , could load a large number of Pd-Ag HDs to enhance the sensitivity and amplify the signal of the immunosensor. Moreover, the electroplated gold nanoparticles (Au NPs) were employed for the immobilization of primary antibodies (Ab 1 ). Au NPs with excellent conductivity could enhance the electron transport between substrate material and electrode surface , and improve the sensitivity of immunosensor. Under optimal conditions, the electrochemical immunosensor exhibited a wide linear range of 0.1 pg/mL–30 ng/mL towards PSA, and a low detection limit of 0.03 pg/mL (S/N = 3). The proposed immunosensor exhibited good sensitivity, reproducibility and stability for the quantitative detection of PSA, which hold a great potential in clinical and diagnostic applications.
研究领域:
生物医学工程
·
分析化学
✓ 已验证
DOI
高影响因子
Science Advances
·
2019
·Vol. 5
·期 1
·
IF 12.804
Hengwei Wang,Xiang-Kui Gu,Xusheng Zheng,Haibin Pan,Junfa Zhu,Si Chen,Lina Cao,Wei-Xue Li,Junling Lu
The prominent size effect of metal nanoparticles shapes decisively nanocatalysis, but entanglement of the corresponding geometric and electronic effects prevents exploiting their distinct functionalities. In this work, we demonstrate that in palladium (Pd)–catalyzed aerobic oxidation of benzyl alcohol, the geometric and electronic effects interplay and compete so intensively that both activity and selectivity showed in volcano trends on the Pd particle size unprecedentedly. By developing a strategy of site-selective blocking via atomic layer deposition along with first principles calculations, we disentangle these two effects and unveil that the geometric effect dominates the right side of the volcano with larger-size Pd particles, whereas the electronic effect directs the left of the volcano with smaller-size Pd particles substantially. Selective blocking of the low-coordination sites prevents formation of the undesired by-product beyond the volcano relationship, achieving a remarkable benzaldehyde selectivity and activity at the same time for 4-nm Pd. Disentangling the geometric and electronic effects of metal nanoparticles opens a new dimension for rational design of catalysts.
研究领域:
催化化学
·
纳米材料科学
·
物理化学
·
表面科学
·
分子催化
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DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2016
·
IF 3.205
Qiao Wang,Zhiquan Liu,Wei Wang,Dongmei Liu,Wenxin Shi,Jiaojie He,Penghui Shao,Ruisha Shi,Fuyi Cui
“Mass transfer in catalyst supports”and “reactive sites”are two critical factors for supported thin film catalysts. Based on such considerations, paper composed of cellulose fibers (CFs) is chosen as a competent nano-catalyst carrier because its broad porous structure is conducive to mass transfer. Then a facile aquatic synergistic synthesis is developed to decorate polypyrrole (PPy) encapsulated palladium nano-composites onto the CF paper structures. The pyrrole monomers (Py) reduce Pd 2+ to Pd nanoparticles in aqueous solution, and meanwhile the Pd 2+ initiates the polymerization of Py to PPy. In the as-prepared composite paper catalysts, the broad pores constructed by the microfibers facilitate the reactant diffusion and the Pd/PPy nanoparticles supported on the fibers provide more reactive sites for catalysis. As a result, the catalytic activity for hydrolysis of ammonia borane is improved. The H 2 turnover frequency is 21.1 mol H 2 mol Pd −1 min −1 , surpassed most other Pd based film catalysts. Importantly, excellent stability and reproducibility are also realized by the immobilization of Pd NPs by PPy layers onto fibers.
研究领域:
材料科学
·
纳米技术
·
催化化学
·
能源材料
·
功能高分子
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DOI
高影响因子
Catalysts
·
2016
·Vol. 6
·期 12
·181
·
IF 2.964
Jiahuan Yu,An Shen,Yucai Cao,Guanzhong Lu
A highly efficient and stable Pd-diimine@SBA-15 catalyst was successfully prepared by immobilizing Pd onto diimine-functionalized mesoporous silica SBA-15. With the help of diimine functional groups grafted onto the SBA-15, Pd could be anchored on a support with high dispersion. Pd-diimine@SBA-15 catalyst exhibited excellent catalytic performance for the Suzuki coupling reaction of electronically diverse aryl halides and phenylboronic acid under mild conditions with an ultralow amount of Pd (0.05 mol % Pd). When the catalyst amount was increased, it could catalyze the coupling reaction of chlorinated aromatics with phenylboronic acid. Compared with the catalytic performances of Pd/SBA-15 and Pd-diimine@SiO2catalysts, the Pd-diimine@SBA-15 catalyst exhibited higher hydrothermal stability and could be repeatedly used four times without a significant decrease of its catalytic activity.
研究领域:
催化化学
·
材料化学
·
有机合成
·
纳米材料
·
绿色化学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2016
·
IF 8.328
Junlong Zhang,Yan Lu,Lei Ge,Changcun Han,Yujing Li,Yangqin Gao,Songsong Li,Hao Xu
Novel AuPd bimetallic alloy nanoparticles (NPs) decorated two-dimensional (2D) BiVO 4 nanosheet photocatalysts were successfully synthesized via mild wet-chemical process and facile deposition procedure. The composite photocatalysts were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electronic microscope (TEM), X-ray photoelectron spectroscopy (XPS), UV–vis diffuse reflection spectroscopy (DRS), electron spin resonance (ESR) and surface photovoltage spectroscopy (SPV). The 1.0 wt% AuPd/BiVO 4 nanosheets showed highest photocatalytic activity for the degradation of Rhodamine B (RhB) under visible light (300 W Xe lamp coupled with a UV-cutoff filter (λ ≥ 400 nm)), and the photocatalytic efficiency was improved for about 21.9 and 6.1 times as compared to that of pure BiVO 4 and 1.0 wt% Au/BiVO 4 , respectively. The novel AuPd/BiVO 4 composites may make a way to synthesize 2D semiconductor composites with potential applications for solar energy conversion and environmental purifications.
研究领域:
材料科学
·
光催化
·
纳米材料
·
环境净化
·
能源化学
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
·
2015
·Vol. 3
·期 16
·8659-8666
·
IF 7.443
Yongji Xin,Linen Wu,Lei Ge,Changcun Han,Yujing Li,Siman Fang
In this work, a novel AuPd bimetallic nanoalloy decorated ultrathin 2D titanium dioxide (TiO2) nanosheet with high H2 evolution activity was prepared via a facile in situ synthesis method. The physical and photophysical properties of the as-prepared AuPd/TiO2 nanosheets were characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), UV-visible diffuse reflection spectroscopy (DRS), X-ray photoelectron spectroscopy (XPS), electron spin resonance (ESR) and surface photocurrent spectroscopy (SPC). The photocatalytic H2 evolution experiments indicate that the AuPd co-catalysts can efficiently promote the separation of photogenerated charge carriers in TiO2, and consequently enhance the H2 evolution activity. The 0.3 wt% AuPd/TiO2 sample shows the highest catalytic activity, and the corresponding H2 evolution rate is 526 μmol h−1 g−1, which is 31 times higher than that of pure TiO2 under simulated sunlight (λ > 300 nm) irradiation. A possible mechanism of the enhanced simulated sunlight catalytic performance of AuPd bimetallic nanoparticle (NP) decorated TiO2 nanosheets is proposed to guide further improvement of desirable functional materials. It is expected that the AuPd decorated TiO2 nanosheets obtained via a simple synthesis approach can be used as efficient photocatalysts and exhibit promising potential for new energy applications.
研究领域:
材料科学
·
光催化
·
纳米材料
·
能源化学
·
半导体物理
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）