Catalysts
·
2023
·Vol. 13
·期 2
·435
·
IF 3.9
Yiran Liu,Yao Chen,Wen Guan,Yu Cao,Fang Wang,Yunlei Zhang
Aerobic oxidation of bio-sourced 2,5-bis(hydroxymethyl)furan (BHMF) to 2, 5-furandicarboxylic acid (FDCA), a renewable and green alternative to petroleum-derived terephthalic acid (TPA), is of great significance in green chemicals production. Herein, hierarchical porous bowl-like nitrogen-rich (nitrated) carbon-supported bimetallic Au-Pd nanocatalysts (AumPdn/ N-BNxC) with different nitrogen content and bimetal nanoparticle sizes were developed and employed for the highly efficient aerobic oxidation of BHMF to FDCA in sodium carbonate aqueous solution. The reaction pathway for catalytic oxidation of BHMF went through the steps of BHMF→HMF→HMFCA→FFCA→FDCA. Kinetics studies showed that the activation energies of BHMF, HMF, HMFCA, and FFCA were 58.1 kJ·moL−1, 39.1 kJ·moL−1, 129.2 kJ·moL−1, and 56.3 kJ·moL−1, respectively, indicating that the oxidation of intermediate HMFCA to FFCA was the rate-determining step. ESR tests proved that the active species was a superoxide radical. Owing to the synergy between the nitrogen-rich carbon support and bimetallic Au-Pd nanoparticles, the Au1Pd1/N-BN2C nanocatalysts exhibited BHMF conversion of 100% and FDCA yield of 95.8% under optimal reaction conditions. Furthermore, the nanocatalysts showed good stability and reusability. This work provides a versatile strategy for the design of heterogeneous catalysts for the highly efficient production of FDCA from BHMF.Keywords:2,5-bis(hydroxymethyl)furan;2,5-furandicarboxylic acid;aerobic oxidation;nitrogen-doped carbon;bimetallic Au-Pd nanoparticles
✓ 已验证
产品关联
DOI
高影响因子
Journal of CO2 Utilization
·
2018
·
IF 5.503
Yu-Nong Li,Xiao-Fang Liu,Liang-Nian He
The oxazolidinone as one kind of annular CO 2 derivatives has been hydrogenated by a new catalytic system Pd/C-TMGPEG 150 Me (polyethylene glycol-functionalized 1,1,3,3-tetramethyl guanidine), affording two valuable products i.e. formic acid and the corresponding secondary alkyl-(2-arylethyl)amines in the high yields of 89% and 98%, respectively. This hydrogenation can be carried out smoothly under relatively mild conditions of 60 °C, 4 MPa of H 2 with a liquid/solid carbon source (oxazolidinone) instead of high pressure CO 2 . The notable results can be successfully obtained even at room temperature under atmospheric H 2 pressure. This one stone two bird strategy is applicable to series of 5-aryl-2-oxazolidinones and opens up a novel way of synthesizing linear secondary alkyl-(2-arylethyl)amines without the selectivity issues, and validates a potential alternative approach for indirect conversion of CO 2 to energy-related products formic acid, as oxazolidinones can be readily obtained from hydrogenation of CO 2 .
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2018
·
IF 6.759
Juan Du,Jiaren Zhang,Yong Sun,Wenlong Jia,Zhihao Si,He Gao,Xing Tang,Xianhai Zeng,Tingzhou Lei,Shijie Liu,Lu Lin
Catalytic transfer hydrogenation (CTH) of bio-derived furfural (FF) to furfuryl alcohol (FFA) was performed using the physically mixed CuO-Pd/C as catalyst and formic acid (FA) as hydrogen donor. The evolution investigation of Cu showed the precursor CuO firstly dissolved into Cu 2+ by FA and then formed coordination polymer-copper(II), which uniformly dispersed in reaction solution of 1, 4-dioxane. Subsequently the Cu 2+ was in-situ reduced and Cu-Pd alloys formed simultaneously. The in-situ prepared nano Cu-Pd/C catalyst exhibited the best performance with a complete FF conversion and FFA selectivity of 98.1%. Reaction conditions test suggested that the FFA selectivity was greatly dependent on the Cu content. The underlying mechanism revealed that the Pd in Cu-Pd alloys mainly promoted the FF conversion by enhancing hydrogen adsorption, while the nano Cu for increasing FFA selectivity; the Cu-Pd alloys functioned in synergistic way. Leaching and recycling tests demonstrated an excellent stability of the Cu-Pd/C catalyst.
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2016
·
IF 7.145
Maoqiang Chi,Guangdi Nie,Yanzhou Jiang,Zezhou Yang,Zhen Zhang,Ce Wang,Xiaofeng Lu
Here, we report a simple one-step procedure to fabricate coaxial Te@poly(3,4-ethylenedioxythiophene) (PEDOT) nanocables via a self-assembly redox polymerization between 3,4-ethylenedioxythiophene monomer and the oxidant of sodium tellurite without the assistance of any templates and surfactants. The as-synthesized Te@PEDOT coaxial nanocables have diameters of center cores in the range of 5–10 nm, and the size of the outer shell from several nanometers to 15 nm. More interestingly, the as-prepared Te@PEDOT nanocables can be converted to Pd@PEDOT nanocables via a galvanic replacement reaction. The center core of the Pd nanowire exhibits a high crystallinity. The application of the synthesized Pd@PEDOT nanocables as peroxidase-like catalysts for the colorimetric detection of H2O2 is reported. The synergistic effect between the Pd nanowire and electrically conducting PEDOT enhances the catalytic activity toward the oxidation of the peroxidase substrate 3,3′,5,5′-tetramethylbenzidine in the presence of H2O2. A detection limit toward H2O2 is as low as 4.83 μM, and a linear range from 10 to 100 μM has been achieved. This work offers a potential versatile route for the fabrication of cable-like nanocomposites with conducting polymers and other active components, which display great promise in applications such as catalysis, nanoelectronic devices, and energy storage and conversion.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Catalysis Science & Technology
·
2015
·Vol. 6
·期 3
·869-874
·
IF 5.426
Shu-Tao Gao,Weihua Liu,Cheng Feng,Ning-Zhao Shang,Chun Wang
Highly dispersed Ag–Pd alloys deposited on an amine-functionalized UiO-66(NH2–UiO-66) have been successfully prepared via a pre-coordination method. The as-synthesized AgPd@NH2–UiO-66 catalyst exhibited 100% H2 selectivity and a high catalytic activity (TOF = 103 h−1) toward the dehydrogenation of formic acid at room temperature without any additives, which is among the highest values ever reported. Our study further reveals that the synergetic effect between the Ag–Pd alloy and NH2–UiO-66 support play a key role for the efficient catalytic dehydrogenation of formic acid.
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL RESEARCH
·
2024
·
IF 7.7
Zihao Li,Zewen Chen,Chen Ye,Lixi Gong,Hui Wang,Jie Zhou
Despite the low cost of supported non-precious metal catalysts, their catalytic activity is significantly lower than that of precious metal catalysts in the catalytic oxidation reaction of volatile organic compounds (VOCs). In order to enhance the catalytic activity of supported non-precious metal catalysts, we introduced an ultra-low loading of palladium into the existing catalytic system and employed a plasma preparation process instead of the conventional impregnation method. The approach significantly improves the catalytic activity of the active sites on the catalyst. The results indicate that, compared to the supported Pd and CuMnCeO x catalysts prepared by conventional impregnation method, the Pd/CuMnCeO x /SiO 2 -P catalysts prepared via plasma exhibit a higher proportion of lattice defects (oxygen vacancies). Furthermore, the doping of the ultra-low Pd could facilitate the formation of additional lattice defects in the composite oxide. As a result, it can improve the content of surface active oxygen and enhance the adsorptive strength of hexane on the surface of the catalyst. The Pd/CuMnCeO x /SiO 2 -P catalysts exhibit high catalytic activity and stability in the catalytic oxidation of n-hexane. This work promotes the potential application in the preparation of catalyst with ultra-low precious metal loading.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Xingjie Guo,Ge Gao,Javier Remón,Ya Ma,Zhicheng Jiang,Bi Shi,Daniel C.W. Tsang
Food waste worldwide has been threatening the environment and resulting in high carbon emissions. Although anaerobic fermentation is a potential solution transforming food waste into valuable chemicals, a large amount of the fermentation residue remains as solid waste. For closing the circular economy loop for food waste valorization, we proposed a thermo-chemical activation of a fermentation residue produced from a mixture of food waste and sludge to prepare a nitrogen-enriched, advanced carbon material. This could be used as a support to synthesize Pd/C, Pt/C and Au/C catalysts for the aqueous-phase hydrogenation of vanillin to vanillyl alcohol at mild reaction conditions. The produced alcohol increased sixfold the commercial value of the original aldehyde. The catalytic performance (based on the vanillin conversion and vanillyl alcohol yield) followed the order of Pd/C > Pt/C > Au/C. The Pd/C catalyst showed an excellent catalytic activity (>99% vanillin conversion and > 99% vanillyl alcohol selectivity) at optimized reaction conditions (i.e., 30 °C and 0.7 MPa H 2 for 90 min, with 2 mmol vanillin/10 mg catalyst), along with high reusability and stability (up to four consecutive runs). These catalytic features outperformed those of a commercial Pd/C catalyst owing to: (i) high reduction degree and stabilization of the Pd particles on the carbon support, which accommodated a higher proportion of pyridinic than pyrrolic nitrogen, and (ii) rapid adsorption of the aldehyde group on the catalyst combined with rapid desorption of the newly formed hydroxymethyl group. This exceptional catalytic behavior was corroborated by efficient hydrogenation of other lignin-derived aromatic aldehydes, including p-hydroxybenzaldehyde and syringaldehyde, to their respective alcohols. Our results can bring a novel use for food waste in catalysis and represent a sustainable and efficient conversion of biomass into value-added chemicals and advanced materials.
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2025
·
IF 4.8
Kaihao Li,Yongwang Li,Yang Qin,Zheng Wang,Bingxin Zhu,Yancong Yin,Fumin Wang,Xubin Zhang
The production of high-purity hydrogen chloride from petrochemical by-product hydrogen chloride gas represents the primary industrial approach for manufacturing electronic-grade hydrogen chloride. However, trace acetylene and ethylene impurities in the feedstock severely compromise product quality. This study innovatively proposes a "stepwise conversion-deep chlorination" synergistic mechanism and successfully develops a bimetallic catalyst (10 %Fe/0.5 %Pd/AC). By tailoring the preparation processes, we precisely controlled the distribution of Fe and Pd active sites, while systematically comparing the performance between Single-metal tandem catalytic system (Pd/AC + Fe/AC) and the bimetallic catalyst. Experimental results combined with DFT calculations demonstrate the superior performance of the 10 %Fe/0.5 %Pd/AC catalyst and confirm the cascade reaction mechanism based on the synergistic tandem effect of Fe/Pd active sites: Acetylene preferentially undergoes hydrochlorination at Pd sites to form vinyl chloride, while ethylene and the resultant vinyl chloride are subsequently converted to chloroethane and more easily removable 1,1-dichloroethane at Fe sites. Under optimized conditions (120 °C, GHSV=180 h −1 ), removal efficiencies exceeding 99 % for both acetylene and ethylene were achieved, with 1,1-dichloroethane selectivity surpassing 99 %. Comprehensive characterizations demonstrated the outstanding stability of the 10 %Fe/0.5 %Pd/AC catalyst. This study presents an innovative catalytic approach for high-efficiency purification of industrial hydrogen chloride.
✓ 已验证
产品关联
DOI
高影响因子
Coatings
·
2025
·Vol. 15
·期 9
·1027
·
IF 2.8
Minglei Yang,Zhenhong Xu,Chongjun Tang,Shuaijie Wang,Zhourong Xiao,Fei Ye
This research introduces a synergistic photoelectrocatalytic (PEC) system designed for the effective degradation of tetracycline (TC), integrating a PO43−-grafted Mo-doped BiVO4(PO43−-Mo:BiVO4) photoanode with a Pd-loaded ordered mesoporous carbon (Pd/CMK-3) cathode. The incorporation of Mo doping and PO43−modification significantly improved the photoanode’s charge separation efficiency, achieving a photocurrent density of 2.9 mA cm−2, and fine-tuned its band structure to enhance hydroxyl radical (·OH) generation. Meanwhile, the Pd/CMK-3 cathode promoted a two-electron oxygen reduction reaction pathway, producing hydrogen peroxide (H2O2) and facilitating molecular oxygen activation via atomic hydrogen (H*) intermediates. Under optimized conditions—1.0 V vs. Ag/AgCl of anodic potential, pH 6.58, and oxygen saturation—the combined system accomplished 80% TC degradation within 60 min, markedly surpassing the performance of the photoanode (72%) or cathode (71%) alone. Notably, this synergistic approach also reduced energy consumption to 0.0065 kWh m−3, outperforming individual components. Radical quenching experiments and liquid chromatography–mass spectrometry (LC-MS) analysis revealed that the photogenerated holes (h+) and ·OH were the key reactive species responsible for TC mineralization. The system demonstrated remarkable stability, with only a 2.96% decline in activity, and effectively degraded other contaminants, such as phenol, 4-chlorophenol, and ciprofloxacin. This study highlights an energy-efficient PEC strategy that harnesses the combined strengths of anodic oxidation and cathodic molecular oxygen activation to significantly enhance the removal of organic pollutants.
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2024
·
IF 7.7
Aowei Lv,Xue Lv
Anthropogenic wastewater generation and water pollution can have negative impacts on public health and ecosystems. However, most materials do not have both adsorptive and catalytic properties, so the design and development of sustainable and multifunctional materials is essential for wastewater treatment. Herein, composite hydrogel (PHG) containing [2-(Methacryloyloxy)ethyl]dimethyl-(3-sulfopropyl) ammonium hydroxide (SBMA) and chitosan quaternary ammonium salts (HACC) were prepared for wastewater treatment. The adsorption capacities of the PHG hydrogels for nickel (Ni II ), copper (Cu II ), and palladium (Pd II ) ions were 158.68, 182.99, and 229.78 mg/g, respectively. The adsorption process is consistent with the Langmuir adsorption model and quasi-secondary kinetics. For further application of adsorbed metal ions, NaBH 4 was selected for in situ reduction to prepare hydrogel-based catalysts cemented with metal nanoparticles (Ni-, Cu- and Pd-NPs), respectively. The PHG-Pd catalysts demonstrated significant catalytic efficiency in reducing 4-nitrophenol and methylene blue, and K app were 0.307 and 0.365 min −1 , respectively. Among them, the activation parameters for the reduction of 4-NP over PHG-Pd catalyst were calculated as E a = 36.27 kJ/mol, ΔH # = 33.72 kJ/mol and ΔS # = −259.68 J/(mol·K). This study is expected to provide insights into the design of multifunctional adsorption catalysts for the removal of dyes and nitro compounds from wastewater.
✓ 已验证
产品关联
DOI
PubMed
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.
✓ 已验证
DOI
高影响因子
Catalysis Science & Technology
·
2018
·Vol. 9
·期 2
·286-301
·
IF 5.365
Mengyuan Zhang,Shipeng Wu,Longchun Bian,Qiue Cao,Wenhao Fang
Ce–Ni mixed oxides with different Ni/Ce molar ratios, promoted by a rather low amount of Pd (0.2 wt%), were prepared by a simple one-pot precipitation method. The thus-synthesized CeNiXOY and Pd–CeNiXOY catalysts were applied respectively to the direct N-alkylation of amine and alcohol via oxidative coupling, under O2 in the absence of basic additives. The CeNiXOY catalyst could provide a >99% yield of imine in the model alkylation reaction of aniline with benzyl alcohol at 100 °C. The Pd-promoted Pd–CeNiXOY catalyst surprisingly showed an enhanced imine yield (>99%) at a mild temperature of 60 °C. This catalyst exhibited good reusability, and moreover, demonstrated high performance towards imine synthesis from various amines with alcohols. The presence of Pd species and the Ni/Ce molar ratio showed a synergistic impact on the conversion of aniline, as well as on the product selectivity, which was believed to be related to the improvement on the intrinsic activity of the oxidation of benzyl alcohol to benzaldehyde. Various physicochemical techniques, including ICP-MS, XRD, N2 adsorption–desorption, UV-Raman, H2-TPR, TEM, EPMA and XPS, were employed to study mainly the composition, structure and redox properties of the catalysts. The proportion of Ce3+ species and oxygen vacancies, which can be manipulated by the Ce–Ni redox system and the interaction between Ce and Ni, was crucial to the selective activation of alcohols in the presence of reactive amines. The activation of alcohol on the highly reactive Pd0 species was the other crucial factor.
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）