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Robust Co-catalytic Performance of Nanodiamonds Loaded on WO3 for the Decomposition of Volatile Organic Compounds under Visible Light

MetadataDetails
Publication Date2016-11-17
JournalACS Catalysis
AuthorsHyoung‐il Kim, Hee-na Kim, Seunghyun Weon, Gun‐hee Moon, Jae‐Hong Kim
InstitutionsPohang University of Science and Technology, Yale University
Citations114
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Technical Documentation and Analysis: Nanodiamond Co-Catalysis for Advanced Photocatalysis

Section titled “Technical Documentation and Analysis: Nanodiamond Co-Catalysis for Advanced Photocatalysis”

This documentation analyzes the application of Nanodiamonds (NDs) as a cost-effective, robust co-catalyst for visible-light-driven photocatalytic decomposition of Volatile Organic Compounds (VOCs), offering a direct replacement strategy for expensive noble metals like Platinum (Pt) and Palladium (Pd).

  • Core Achievement: Nanodiamonds loaded onto Tungsten Oxide (ND/WO3) demonstrate superior photocatalytic activity, achieving VOC degradation rates approximately 17 times higher than bare WO3 under visible light (Îť > 420 nm).
  • Performance Benchmark: The activity of optimal ND/WO3 is directly comparable to or slightly lower than the expensive benchmark, Pt/WO3 (ka ND/WO3 = 5.16 x 10-2 min-1 vs. ka Pt/WO3 = 6.05 x 10-2 min-1).
  • Mechanism Insight: The efficacy is attributed to the unique spÂł (diamond core)/sp² (graphitic shell) structure of the NDs, where the conductive graphitic surface shell facilitates enhanced charge separation and interfacial electron transfer, acting as a Pt-like co-catalyst.
  • Cost Efficiency: NDs, being Earth-abundant carbon materials, are proposed as a scalable, inexpensive, and practical alternative to high-cost noble metals for environmental remediation and air purification systems.
  • Stability & Scalability: The hybrid ND/WO3 photocatalyst demonstrated excellent stability over repeated cycles and minimizes light-shielding issues common in other carbon-based co-catalysts (e.g., graphene).

The following hard data points were extracted detailing the performance and physical properties of the optimized photocatalyst systems.

ParameterValueUnitContext
Optimal ND Loading8wt%Maximum ka for Acetaldehyde degradation
WO3 Bandgap (Eg)2.8eVBase material utilizes visible light
Light Source WavelengthÎť > 420nmVisible light irradiation regime
ND/WO3 Kinetic Rate Constant (ka)5.16 x 10-2min-1Under visible light (Îť > 420 nm)
Pt/WO3 Kinetic Rate Constant (ka)6.05 x 10-2min-1Benchmark performance (1 wt% Pt)
Bare WO3 Kinetic Rate Constant (ka)0.30 x 10-2min-1Demonstrates 17x enhancement by ND loading
Acetaldehyde Removal (ND/WO3)92.1%After 1 hour of reaction
Acetaldehyde Oxidation Yield (ND/WO3)65.7%Conversion to CO2 + H2O
Initial Acetaldehyde Concentration100ppmvModel VOC concentration
Nanodiamond Particle Size4-6nmDiameter of precursor material (uDiamond Allegro)
Hydrogen Treatment Temperature800°CFor H-Ox-NDs (restoring surface conductivity)

The robust catalytic performance hinges on specific material preparation and modification techniques, critical for controlling the diamond surface chemistry.

  1. Nanodiamond Precursor: Commercial Nanodiamond solution (uDiamond Allegro, ca. 5 wt%, 4-6 nm diameter) was filtered and rinsed to obtain ND powder.
  2. Surface Functionalization (Modifying sp²/sp³ Ratio):
    • Oxidized NDs (Ox-NDs): Obtained via annealing NDs at 430 °C for 5 h under air (removes conductive sp² layer).
    • Hydrogenated Ox-NDs (H-Ox-NDs): Prepared by annealing Ox-NDs at 800 °C for 2 h under H2 flow (restores surface conductivity).
    • Graphitized NDs (G-NDs): Prepared by annealing NDs at 1200 °C for 2 h under Argon flow (increases sp² thickness).
  3. Catalyst Loading (ND/WO3): ND powder was dispersed in water, and WO3 (Aldrich) was added. The NDs were loaded onto WO3 surfaces via a simple dehydration condensation method between oxygen-containing functional groups (on NDs) and hydroxyl groups (on WO3).
  4. Film Preparation: Photocatalyst paste (0.15 g mL-1 in ethanol) was spread onto 40 mm x 20 mm plate glass slides using a doctor blade method and annealed at 200 °C under argon flow.
  5. Activity Measurement: VOC degradation (Acetaldehyde, Toluene) and concurrent CO2 production were monitored in a closed-circulation Pyrex reactor (300 cmÂł) under visible light (Îť > 420 nm, 18 mW cm-2).
  6. Mechanistic Analysis: Photoelectrochemical (PEC) measurements (slurry and electrode-type) and characterization techniques (HR-TEM, XPS, Raman) were used to confirm electron transfer pathways and the critical role of the ND graphitic surface layer.

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Cost-Effective Noble Metal ReplacementScalability via Large-Area MPCVD: By confirming NDs as an effective alternative to Pt/Pd, 6CCVD’s capability to grow large-area PCD plates (up to 125mm) and thick substrates (up to 10mm) enables the development of scalable, industrial-grade photocatalytic reactors that leverage abundant carbon materials instead of expensive noble metals.
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View Original Abstract

Proper co-catalysts (usually noble metals), combined with semiconductor materials, are commonly needed to maximize the efficiency of photocatalysis. Search for cost-effective and practical alternatives for noble-metal co-catalysts is under intense investigation. In this work, nanodiamond (ND), which is a carbon nanomaterial with a unique sp(3)(core)/sp(2)(shell) structure, was combined with WO3 (as an alternative co-catalyst for Pt) and applied for the degradation of volatile organic compounds under visible light. NDs-loaded WO3 showed a highly enhanced photocatalytic activity for the degradation of acetaldehyde (similar to 17 times higher than bare WO3), which is more efficient than other well-known co-catalysts (Ag, Pd, Au, and CuO) loaded onto WO3 and comparable to Pt-loaded WO3. Various surface modifications of ND and photoelectochemical measurements revealed that the graphitic carbon shell (sp(2)) on the diamond core (spa) plays a crucial role in charge separation and the subsequent interfacial charge transfer. As a result, ND/WO3 showed much higher production of OH radicals than bare WO3 under visible light. Since ND has a highly transparent characteristic, the light shielding that is often problematic with other carbon-based co-catalysts was considerably lower with NDs-loaded WO3. As a result, the photocatalytic activity of NDs/WO3 was higher than that of WO3 loaded with other carbon-based co-catalysts (graphene oxide or reduced graphene oxide). A range of spectroscopic and photo(electro)chemical techniques were systematically employed to investigate the properties of NDs-loaded WO3. ND is proposed as a cost-effective and practical nanomaterial to replace expensive noble-metal co-catalysts.