Allen Puente-Urbina

Mr. Allen Puente-Urbina

orcid

Research Focus & Metrics

Academic Career Length

11Years (2016-Present)

(Calculated once Scilit publication data is synced: current year − year of first publication + 1)

Representative Publications

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23 August 2024 in Science
Verified
Journal Article
Closed access
RCRyan W. Clarke
Ryan W. Clarke
ERErik G. Rognerud
Erik G. Rognerud
APAllen Puente-Urbina
Allen Puente-Urbina
DBDavid Barnes
David Barnes
Paul MurdyPaul Murdy
Paul Murdy
NRNicholas A. Rorrer
Nicholas A. Rorrer
Wind energy is helping to decarbonize the electrical grid, but wind blades are not recyclable, and current end-of-life management strategies are not sustainable. To address the material recyclability challenges in sustainable energy infrastructure, we introduce scalable biomass-derivable polyester covalent adaptable networks and corresponding fiber-reinforced composites for recyclable wind blade fabrication. Through experimental and computational studies, including vacuum-assisted resin-transfer molding of a 9-meter wind blade prototype, we demonstrate drop-in technological readiness of this material with existing manufacture techniques, superior properties relative to incumbent materials, and practical end-of-life chemical recyclability. Most notable is the counterintuitive creep suppression, outperforming industry state-of-the-art thermosets despite the dynamic cross-link topology. Overall, this report details the many facets of wind blade manufacture, encompassing chemistry, engineering, safety, mechanical analyses, weathering, and chemical recyclability, enabling a realistic path toward biomass-derivable, recyclable wind blades.

18 February 2021 in Chemical Science
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Journal Article
Open access
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ZPZeyou Pan
Zeyou Pan
APAllen Puente-Urbina
Allen Puente-Urbina
ABAndras Bodi
Andras Bodi
JBJeroen A. van Bokhoven
Jeroen A. van Bokhoven
PHPatrick Hemberger
Patrick Hemberger
The catalytic pyrolysis mechanism of the initial lignin depolymerization products will help us develop biomass valorization strategies. How does isomerism influence reactivity, product formation, selectivities, and side reactions? By using imaging photoelectron photoion coincidence (iPEPICO) spectroscopy with synchrotron radiation, we reveal initial, short-lived reactive intermediates driving benzenediol catalytic pyrolysis over H-ZSM-5 catalyst. The detailed reaction mechanism unveils new pathways leading to the most important products and intermediates. Thanks to the two vicinal hydroxyl groups, catechol (o-benzenediol) is readily dehydrated to form fulvenone, a reactive ketene intermediate, and exhibits the highest reactivity. Fulvenone is hydrogenated on the catalyst surface to phenol or is decarbonylated to produce cyclopentadiene. Hydroquinone (p-benzenediol) mostly dehydrogenates to produce p-benzoquinone. Resorcinol, m-benzenediol, is the most stable isomer, because dehydration and dehydrogenation both involve biradicals owing to the meta position of the hydroxyl groups and are unfavorable. The three isomers may also interconvert in a minor reaction channel, which yields small amounts of cyclopentadiene and phenol via dehydroxylation and decarbonylation. We propose a generalized reaction mechanism for benzenediols in lignin catalytic pyrolysis and provide detailed mechanistic insights on how isomerism influences conversion and product formation. The mechanism accounts for processes ranging from decomposition reactions to molecular growth by initial polycyclic aromatic hydrocarbon (PAH) formation steps to yield, e.g., naphthalene. The latter involves a Diels–Alder dimerization of cyclopentadiene, isomerization, and dehydrogenation.

27 July 2023 in Nature Communications
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Journal Article
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ZPZeyou Pan
Zeyou Pan
APAllen Puente-Urbina
Allen Puente-Urbina
SBSyeda Rabia Batool
Syeda Rabia Batool
ABAndras Bodi
Andras Bodi
XWXiangkun Wu
Xiangkun Wu
PHPatrick Hemberger
Patrick Hemberger
Unveiling catalytic mechanisms at a molecular level aids rational catalyst design and selectivity control for process optimization. In this study, we find that the Brønsted acid site density of the zeolite catalyst efficiently controls the guaiacol catalytic pyrolysis mechanism. Guaiacol demethylation to catechol initiates the reaction, as evidenced by the detected methyl radicals. The mechanism branches to form either fulvenone (c-C5H4 = C = O), a reactive ketene intermediate, by catechol dehydration, or phenol by acid-catalyzed dehydroxylation. At high Brønsted acid site density, fulvenone formation is inhibited due to surface coordination configuration of its precursor, catechol. By quantifying reactive intermediates and products utilizing operando photoelectron photoion coincidence spectroscopy, we find evidence that ketene suppression is responsible for the fivefold phenol selectivity increase. Complementary fulvenone reaction pathway calculations, along with 29Si NMR-MAS spectroscopy results corroborate the mechanism. The proposed, flexible operando approach is applicable to a broad variety of heterogeneous catalytic reactions.

18 May 2022 in ChemSusChem
Verified
Journal Article
Open access
ASAmrita Singh‐Morgan
Amrita Singh‐Morgan
APAllen Puente-Urbina
Allen Puente-Urbina
JBJeroen A. van Bokhoven
Jeroen A. van Bokhoven
Lignin is an abundant natural polymer obtained from lignocellulosic biomass and rich in aromatic substructures. When efficiently depolymerized, it has great potential in the production of value‐added chemicals. Fast pyrolysis is a promising depolymerization method, but current studies focus mainly on small quantities of lignin. In this Review, to determine the potential for upscaling, systems used in the most relevant unit operations of fast pyrolysis of lignin are evaluated. Fluidized‐bed reactors have the most potential. It would be beneficial to combine them with the following: slug injectors for feeding, hot particle filters, cyclones, and fractional condensation for product separation and recovery. Moreover, upgrading lignin pyrolysis oil would allow the necessary quality parameters for particular applications to be reached.

29 August 2021 in Angewandte Chemie International Edition
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Journal Article
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APAllen Puente-Urbina
Allen Puente-Urbina
ZPZeyou Pan
Zeyou Pan
VPVladimir Paunović
Vladimir Paunović
PŠPetr Šot
Petr Šot
PHPatrick Hemberger
Patrick Hemberger
JBJeroen Anton van Bokhoven
Jeroen Anton van Bokhoven
Radical‐mediated gas‐phase reactions play an important role in the conversion of methane under non‐oxidative conditions into olefins and aromatics over iron‐modified silica catalysts. Herein, we use operando photoelectron photoion coincidence spectroscopy to disentangle the elusive C2+ radical intermediates participating in the complex gas‐phase reaction network. Our experiments pinpoint different C2‐C5 radical species that allow for a stepwise growth of the hydrocarbon chains. Propargyl radicals (H2C−C≡C−H) are identified as essential precursors for the formation of aromatics, which then contribute to the formation of heavier hydrocarbon products via hydrogen abstraction–acetylene addition routes (HACA mechanism). These results provide comprehensive mechanistic insights that are relevant for the development of methane valorization processes.

21 March 2018 in Energies
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Journal Article
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Johanna Gaitán-ÁlvarezJohanna Gaitán-Álvarez
Johanna Gaitán-Álvarez
Roger Alonso Moya RoqueRoger Alonso Moya Roque
Roger Alonso Moya Roque
APAllen Puente-Urbina
Allen Puente-Urbina
ARAna Rodriguez-Zúñiga
Ana Rodriguez-Zúñiga
We evaluated the thermogravimetric and devolatilization rates of hemicellulose and cellulose, and the calorimetric behavior of the torrefied biomass, of five tropical woody species (Cupressus lusitanica, Dipteryx panamensis, Gmelina arborea, Tectona grandis and Vochysia ferruginea), at three temperatures (TT) and three torrefaction times (tT) using a thermogravimetric analyzer. Through a multivariate analysis of principal components (MAPC), the most appropriate torrefaction conditions for the different types of woody biomass were identified. The thermogravimetric analysis-derivative thermogravimetry (TGA-DTG) analysis showed that a higher percentage of the hemicellulose component of the biomass degrades, followed by cellulose, so that the hemicellulose energy of activation (Ea) was less than that of cellulose. With an increase in TT and tT, the Ea for hemicellulose decreased but increased for cellulose. The calorimetric analyses showed that hemicellulose is the least stable component in the torrefied biomass under severe torrefaction conditions, and cellulose is more thermally stable in torrefied biomass. From the MAPC results, the best torrefaction conditions for calorimetric analyses were at 200 and 225 °C after 8, 10, and 12 min, for light and middle torrefaction, respectively, for the five woody species.