Enhancing Low-Temperature Syngas Production via Surface Tailoring of Supported Intermetallic Nanocatalysts

Johnson, Olusola; He, Yang; Pierre-Charles, Isabella St.; Richter, Jillian; Joseph, Babu; Kuhn, John N.

doi:10.1021/acscatal.4c01180

Title: Enhancing Low-Temperature Syngas Production via Surface Tailoring of Supported Intermetallic Nanocatalysts

Journal Article · 01 May 2024 · ACS Catalysis

DOI: https://doi.org/10.1021/acscatal.4c01180 · OSTI ID:2349423

^[1]; He, Yang ^[2]; Pierre-Charles, Isabella St. ^[3]; Richter, Jillian ^[3]; Joseph, Babu ^[3];

^[3]

University of South Florida, Tampa, FL (United States); University of South Florida
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
University of South Florida, Tampa, FL (United States)

An active and coke-resistant silica-encapsulated intermetallic Ni₃Zn nanoparticle catalyst was developed for low-temperature (450 °C) dry reforming of methane (DRM). The catalyst exhibited a remarkable 4-fold increase in activity (4.5 s^–1) with over 99% CO selectivity and 3 orders of magnitude less carbonaceous species and demonstrated remarkable stability (70 h) compared to that of a monometallic Ni catalyst. Here, the key is the combined effect of surface ensemble structure and electronic interaction modulation through the surface composition tailoring achieved by off-stoichiometric Ni and Zn loading in controlling surface chemistry for achieving different activities and H₂/CO ratios. Characterized by ion spectroscopy, X-ray photoelectron spectroscopy, and the neutron pair distribution function, it was revealed that paired Ni^{δ^–}–Zn^δ+ active sites are crucial for DRM. Transient infrared spectroscopy and isotopic analysis uncovered the synergistic effect of Ni^{δ^–}–Zn^δ+ sites in activating C–H bonds and dissociating CO₂ to prevent coke formation under low-temperature conditions.

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Research Organization:: University of South Florida, Tampa, FL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: EE0008488

OSTI ID:: 2349423

Journal Information:: ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 10 Vol. 14; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Activation energy
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Title: Enhancing Low-Temperature Syngas Production via Surface Tailoring of Supported Intermetallic Nanocatalysts

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