MICROCHIMICA ACTA
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2020
·Vol. 187
·期 11
·1-11
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IF 6.232
Cui Ying,Li Junhua,Liu Mengqin,Tong Haixia,Liu Zeng,Hu Jiawen,Qian Dong
A novel hybrid with three-dimensional (3D) hierarchical CuS@Pd core-shell cauliflowers decorated on nitrogen-doped reduced graphene oxide (CuS@Pd/N–RGO) has been prepared by a facile wet-chemical route without utilizing any template molecules and surfactants. The characterization results reveal that the 3D flower-like structure of CuS “core” is composed of interconnecting nanoplates, which is conductive to the loading of Pd nanoparticles’ “shell” and results in the robust interaction between the core and shell for the formation of CuS@Pd cauliflowers. Anchoring such appealing CuS@Pd cauliflowers on the two-dimensional N–RGO can efficaciously inhibit the aggregation of CuS@Pd cauliflowers and accelerate the kinetics of xanthine oxidation. Benefiting from the multi-functional properties and unique morphology, the sensor constructed by CuS@Pd/N–RGO exhibits excellent performance for non-enzymatic detection of xanthine including a wide detection range of 0.7–200.0 μM (0.94 V vs. SCE), a low detection limit of 28 nM (S/ N = 3), high reproducibility (relative standard deviation (RSD) = 4.1%), and commendable stability (retained 90% of the initial electrochemical responses after storage for 30 days), which is amongst the best of various electrochemical sensors reported for xanthine assays till date. Reliable and satisfying recoveries (95–105%, RSD ≤ 4.1%) are achieved for xanthine detection in real samples. The inspiring results make the uniquely structural CuS@Pd/N–RGO greatly promising in non-enzymatic electrochemical sensing applications.
A high-performance non-enzymatic xanthine sensor has been constructed by the three-dimensional hierarchical CuS@Pd core-shell cauliflowers decorated on nitrogen-doped reduced graphene oxide.
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Journal of CO2 Utilization
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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 .
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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.
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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.
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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.
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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.
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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.
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Journal of Cleaner Production
·
2025
·
IF 10
Tao Jiang,Ming Cheng,Yujiao Wang,Shaoqiang Guo,Wentao Zhou,Yafei Wang
The selective removal of neutron-absorbing fission products from spent nuclear fuel is critical for enhancing neutron economy and enabling efficient recycling. In this work, we present a novel two-step dry reprocessing strategy that integrates NH 3 /HCl gas mixture treatment with liquid Sn extraction to achieve phase-selective separation of Sm, Nd, Ru, Rh, and Pd from simulated U 3 O 8 -based spent fuel. Thermodynamic analysis and experimental validation reveal that decomposition of NH 4 Cl at elevated temperatures serves as the generator of NH 3 /HCl gas mixture capable of selectively chlorinating Sm 2 O 3 and Nd 2 O 3 into soluble chlorides while reducing U 3 O 8 to UO 2 and converting RuO 2 , Rh 2 O 3 , and PdO to their metallic states (Ru, Rh, Pd). Subsequent dissolution tests in LiCl-KCl confirm that Sm and Nd are almost completely removed, with chlorination efficiencies of nearly 100%, while uranium loss can be minimized by controlling direct NH 4 Cl contact. The coupled liquid Sn extraction at 1173 K enabled the recoveries of metallic Rh, Rh, and Pd with a promising extraction efficiency. This integrated approach significantly simplifies the partitioning of key neutron poisons (Sm, Nd, Ru, Rh, Pd) compared to conventional aqueous or pyrochemical routes, reduces secondary waste, and preserves uranium in its UO 2 form.
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LANGMUIR
·
2025
·
IF 3.9
Chen Shen,Binyu Zhang,Haiyong Wang,Mi Luo,Tianhan Zhu,Tianyu Gao,Tong Zhang,Xiaoli Chen,Chenguang Wang
Precise modulation of interfacial electronic structures is crucial for enhancing the catalytic activity and selectivity in heterogeneous catalysis. The electron penetration effect (EPE), involving electron transfer from a metal core through a protective shell to surface active sites, has emerged as an effective strategy for tuning surface electronic properties and promoting catalytic performance. However, controlled manipulation of EPE remains challenging, particularly in regulating the phase structure of the metal core and the characteristics of the encapsulating shell. In this work, nitrogen-doped graphene-coated Ni nanoparticles were synthesized from a Ni-based metal–organic framework (Ni-MOF-T/t) by systematically adjusting the reduction temperature (T) and time (t). Subsequent deposition of Pd species yielded Pd/Ni-MOF-T/t catalysts. Among them, the optimized Pd/Ni-MOF-400 °C/2 h catalyst, featuring a hexagonal Ni core, exhibited enhanced electron penetration across the graphitic shell to the Pd sites, effectively modulating the surface electronic structure and boosting catalytic activity. The catalyst demonstrated excellent performance in both thermocatalytic hydrogenation of benzonitrile (90% conversion, 99.0% selectivity) and electrochemical hydrogenation of 4-nitrophenol (96.5% conversion, 90.5% Faradaic efficiency). These findings highlight that phase-controlled electron penetration provides a versatile and generalizable approach for constructing multifunctional catalysts with superior activity under mild conditions. This work establishes phase engineering of MOF-derived metal–carbon interfaces as an effective strategy to manipulate electron penetration effects and optimize catalytic performance.
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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.
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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.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Xiang Gong,Shuyi Guo,Zhao Jiang,Bolun Yang,Tao Fang
Hydrogen is a promising candidate to substitute the fossil fuels. However, the efficient hydrogen storage technologies restrict the commercial applications. Developing new catalysts with high activity and selectivity is important for the dehydrogenation reaction in N-ethylcarbazole/dodecahydro-N-ethylcarbazole (NECZ/12H-NECZ) hydrogen storage system. In this work, a series of Pd-M/Al 2 O 3 (M = Co, Ni and Cu) bimetallic catalysts are synthesized successfully and show good performance in the dehydrogenation reaction of 12H-NECZ than the commercial Pd/Al 2 O 3 catalyst. The Pd 1 Co 1 /Al 2 O 3 catalyst (Practical Pd content = 2.4136 wt%) showed the highest catalytic performance with 95.34% H 2 release amount, TOF of 230.5 min −1 and 85.4% selectivity of NECZ. Combined with the characterization analysis, it can be proposed that the dehydrogenation performance of 12H-NECZ is dependent on the alloy phases , reasonable electronic structures and nanoparticle size of catalysts. The fine-tuned alloy degree and appropriate nanoparticle size of Pd 1 Co 1 /Al 2 O 3 bring the 17.7% increase of H 2 release amount and 99.5% increase of NECZ selectivity than those of Pd/Al 2 O 3 . For the bimetallic catalysts, the enhancement of selectivity of NECZ is mainly from the increase of the kinetic constant of rate-limiting step.
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