skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.

Explore Research Products in the PAR
It may take a few hours for recently added research products to appear in PAR search results.


Title: Smart paper transformer: new insight for enhanced catalytic efficiency and reusability of noble metal nanocatalysts
Although noble metal nanocatalysts show superior performance to conventional catalysts, they can be problematic when balancing catalytic efficiency and reusability. In order to address this dilemma, we developed a smart paper transformer (s-PAT) to support nanocatalysts, based on easy phase conversion between paper and pulp, for the first time. The pulp phase was used to maintain the high catalytic efficiency of the nanocatalysts and the transformation to paper enabled their high reusability. Herein, as an example of smart paper transformers, a novel chromatography paper-supported Au nanosponge (AuNS/pulp) catalyst was developed through a simple water-based preparation process for the successful reduction of p -nitrophenol to demonstrate the high catalytic efficiency and reusability of the noble metal nanocatalyst/pulp system. The composition, structure, and morphology of the AuNS/pulp catalyst were characterized by XRD, TGA, FE-SEM, ICP, TEM, FT-IR, and XPS. The AuNS/pulp catalyst was transformed into the pulp phase during the catalytic reaction and into the paper phase to recover the catalysts after use. Owing to this smart switching of physical morphology, the AuNS/pulp catalyst was dispersed more evenly in the solution. Therefore, it exhibited excellent catalytic performance for p -nitrophenol reduction. Under optimal conditions, the conversion rate of p -nitrophenol reached nearly 100% within 6 min and the k value of AuNS/pulp (0.0106 s −1 ) was more than twice that of a traditional chromatography paper-based catalyst (0.0048 s −1 ). Additionally, it exhibited outstanding reusability and could maintain its high catalytic efficiency even after fifteen recycling runs. Accordingly, the unique phase switching of this smart paper transformer enables Au nanosponge to transform into a highly efficient and cost-effective multifunctional catalyst. The paper transformer can support various nanocatalysts for a wide range of applications, thus providing a new insight into maintaining both high catalytic efficiency and reusability of nanocatalysts in the fields of environmental catalysis and nanomaterials.  more » « less
Award ID(s):
1827745
PAR ID:
10160756
Author(s) / Creator(s):
; ; ; ; ;
Date Published:
Journal Name:
Chemical Science
Volume:
11
Issue:
11
ISSN:
2041-6520
Page Range / eLocation ID:
2915 to 2925
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. ; ; ; ; ; ; ; ; (, Journal of the American Chemical Society)
    The structural stability of nanocatalysts during electrochemical CO2 reduction (CO2RR) is crucial for practical applications. However, highly active nanocatalysts often reconstruct under reductive conditions, requiring stabilization strategies to maintain activity. Here, we demonstrate that the N-heterocyclic carbene (NHC) polymer stabilizes Au nanowire (NW) catalysts for selective CO2 reduction to CO over a broad potential range, enabling coupling with Cu NWs for one-step tandem conversion of CO2 to C2H4. By combining the hydrophobicity of the polystyrene chain and the strong binding of NHC to Au, the polymer stabilizes Au NWs and promotes CO2RR to CO with excellent selectivity (>90%) across −0.4 V to −1.0 V (vs RHE), a significantly broader range than unmodified Au NWs (−0.5 V to −0.7 V). Stable CO2RR at negative potentials yields a high jCO of 142 A/g Au at −1.0 V. In situ ATR-IR analysis indicates that the NHC polymer regulates the water microenvironment and suppresses hydrogen evolution at high overpotential. Moreover, NHC-Au NWs maintain excellent stability during 10 h of CO2RR testing, preserving the NW morphology and catalytic performance, while unmodified NWs degrade into nanoparticles with reduced activity and selectivity. NHC-Au NWs can be coupled with Cu NWs in a flow cell to catalyze CO2RR to C2H4 with 58% efficiency and a partial current density of 70 mA/cm2 (overall C2 product efficiency of 65%). This study presents an adaptable strategy to enhance the catalyst microenvironment, ensure stability, and enable efficient tandem CO2 conversion into value-added hydrocarbons. 
    more » « less
  2. ; ; (, Materials Research Express)
    Abstract Gold (Au)- and ceria (CeO2)-based catalysts are amongst the most active catalysts for the gas phase CO oxidation reaction. Nevertheless, nanosized Au and CeO2catalysts may encounter heat-induced sintering in thermochemical catalytic reactions. Herein, we report on the rational one-pot synthesis of ceria-reduced graphene oxide (CeO2-RGO) using a facile ethylenediamine (EDA)-assisted solvothermal method. Standalone RGO and free-standing CeO2were also prepared using the same EDA-assisted method for comparison. We then incorporated Au into the prepared samples by colloidal reduction and evaluated the catalytic activity of the different catalysts for CO oxidation. The RGO-supported CeO2surpassed the free-standing CeO2, exhibiting a 100% CO conversion at 285oC compared to 340oC in the case of CeO2. Interestingly, the RGO-supported Au/CeO2catalysts outperformed the Au/CeO2catalysts and achieved a 100% CO conversion at 76oC compared to 113oC in the case of Au/CeO2. Additionally, the Au/CeO2-RGO catalyst demonstrated remarkable room-temperature activity with simultaneous 72% CO conversion. This outstanding performance was attributed to the unique dispersion and size characteristics of the RGO-supported CeO2and Au catalysts in the ternary Au/CeO2-RGO nanocomposite, as revealed by TEM and XPS, among other techniques. 
    more » « less
  3. ; ; (, Molecules)
    In this review, we present an assessment of recent advances in alkyne functionalization reactions, classified according to different classes of recyclable catalysts. In this work, we have incorporated and reviewed the activity and selectivity of recyclable catalytic systems such as polysiloxane-encapsulated novel metal nanoparticle-based catalysts, silica–copper-supported nanocatalysts, graphitic carbon-supported nanocatalysts, metal organic framework (MOF) catalysts, porous organic framework (POP) catalysts, bio-material-supported catalysts, and metal/solvent free recyclable catalysts. In addition, several alkyne functionalization reactions have been elucidated to demonstrate the success and efficiency of recyclable catalysts. In addition, this review also provides the fundamental knowledge required for utilization of green catalysts, which can combine the advantageous features of both homogeneous (catalyst modulation) and heterogeneous (catalyst recycling) catalysis. 
    more » « less
  4. ; ; ; ; ; ; ; ; ; ; et al (, Catalysis Science & Technology)
    Understanding the catalytic oxidation of propane is important for developing catalysts not only for catalytic oxidation of hydrocarbons in emission systems but also for selective oxidation in the chemical processing industry. For palladium-based catalysts, little is known about the identification of the chemical or intermediate species involved in propane oxidation. We describe herein findings of an investigation of the catalytic oxidation of propane over supported palladium nanoalloys with different compositions of gold (Pd n Au 100−n ), focusing on probing the chemical or intermediate species on the catalysts in correlation with the bimetallic composition and the alloying phase structure. In addition to an enhanced catalytic activity, a strong dependence of the catalytic activity on the bimetallic composition was revealed, displaying an activity maximum at a Pd : Au ratio of 50 : 50 in terms of reaction temperature. This dependence is also reflected by its dependence on the thermochemical treatment conditions. While the activity for nanoalloys with n ∼ 50 showed little change after the thermochemical treatment under oxygen, the activities for nanoalloys with n < 50 and n > 50 showed opposite trends. Importantly, this catalytic synergy is linked to the subtle differences of chemical and intermediate species which have been identified for the catalysts with different bimetallic compositions by in situ measurements using diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS). For the catalytic oxidation of propane over the highly-active catalyst with a Pd : Au ratio of 50 : 50, the major species identified include acetate and bicarbonate, showing subtle differences in comparison with the identification of bicarbonate and formate for the catalyst with <50% Au (with a lower activity) and the absence of apparent species for the catalyst with >50% Au (activity is largely absent). The alloying of 50% Au in Pd is believed to increase the oxophilicity of Pd, which facilitates the first carbon–carbon bond cleavage and oxygenation of propane. The implications of the findings on the catalytic synergy of Pd alloyed with Au and the design of active Pd alloy catalysts are also discussed. 
    more » « less
  5. ; ; (, AIChE Journal)
    Abstract This study focused on evaluating the reduction of chlorine content in waste polyvinyl chloride (WPVC) through high‐temperature catalytic hydrothermal treatment (HTT). Catalytic HTT experiments were carried out to evaluate the effect of noble metal catalysts (Ru/C, Pt/C, and Pd/C), residence time (0.5, 1, 2, and, 4 h), reaction temperature (300, 325, and 350°C), and catalyst loading (0, 5, and 10 wt%). The findings indicated that dechlorination efficiency can be achieved by 99.01% at 350°C and 1 h, with 10 wt% Pd/C loading. Based on chlorine balance, the chlorine content of the solid phase significantly decreased from 568.8 to 5.64 g kg−1at the same condition. The catalytic HTT solid residue ash has low chlorine content under most operational conditions. These results suggest that catalytic HTT is an effective method to dechlorinate WPVC as a high‐halogenated waste plastic in order to reduce its harmful effect on the environment. 
    more » « less
  • Citation Formats
  • MLA
  • APA
  • Chicago
  • BibTeX
  • Save / Share this Record
  • Send to Email