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arxiv: 2604.18417 · v1 · submitted 2026-04-20 · ❄️ cond-mat.mtrl-sci

Recognition: unknown

Plasmonic Photocatalysis Enables Selective Oxidative Coupling of Methane with Nitrous Oxide under Ambient Conditions

Serin Lee , Lin Yuan , Elijah Begin , Dali Yang , Cedric Lim , Yirui Arlene Zhang , Lu Ma , Colin Ophus
show 3 more authors
Yi Cui Junwei Lucas Bao Jennifer A. Dionne
Authors on Pith no claims yet

Pith reviewed 2026-05-10 03:54 UTC · model grok-4.3

classification ❄️ cond-mat.mtrl-sci
keywords plasmonic photocatalysismethane conversionnitrous oxideC-C couplingselective oxidationAuPd alloyTiO2 catalystambient conditions
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The pith

A tuned AuPd plasmonic catalyst on TiO2 converts methane and nitrous oxide into C2 and C3 hydrocarbons with 80 percent selectivity under visible light at room temperature.

A machine-rendered reading of the paper's core claim, the machinery that carries it, and where it could break.

The paper shows that a gold-palladium alloy supported on titanium dioxide can drive the reaction of two greenhouse gases into multi-carbon products using only visible light at ambient conditions. Gold improves light absorption while palladium activates the C-H bonds, and the resulting plasmonic hot carriers control the surface intermediates to favor carbon-carbon coupling. A reader would care because conventional routes need temperatures up to 1000 C and still produce substantial CO2, whereas this route suppresses over-oxidation and yields ethylene, ethane, propylene, and propane. The work therefore links light-driven carrier dynamics directly to lowered reaction barriers and improved product distribution.

Core claim

An optimal AuPd0.05 composition on TiO2, illuminated by visible light, produces C2H4, C2H6, C3H6, and C3H8 with roughly 80 percent selectivity while suppressing CO2. In-situ spectroscopy and calculations indicate that plasmon-generated carriers redistribute interfacial hydroxyl intermediates, shifting the surface to suppress overoxidation. Ab-initio results show the C-C coupling barrier drops from 2.7 eV to 0.7 eV under illumination.

What carries the argument

Plasmon-generated hot carriers in the AuPd alloy on TiO2 that redistribute interfacial hydroxyl intermediates to lower C-C coupling barriers.

If this is right

  • Methane and nitrous oxide can be upgraded to multicarbon hydrocarbons without high-temperature reactors or large CO2 coproduction.
  • Interfacial adsorbate redistribution by light-induced carriers can steer selectivity away from complete oxidation toward C-C bond formation.
  • Visible-light illumination can reduce activation barriers for coupling steps by more than 2 eV on suitably engineered metal-oxide interfaces.
  • Systematic alloy composition tuning on oxide supports enables control over both light harvesting and surface chemistry in photocatalysis.

Where Pith is reading between the lines

These are editorial extensions of the paper, not claims the author makes directly.

  • The same carrier-redistribution principle could be tested on other oxide-supported alloys for additional selective C-H activations at mild conditions.
  • If the approach scales, it would lower the energy input needed to convert industrial emissions into higher-value chemicals.
  • Varying illumination intensity while holding temperature fixed would provide a direct experimental test separating electronic from thermal contributions.
  • The hydroxyl-shifting mechanism may apply to related plasmonic systems used for other oxidation or coupling reactions.

Load-bearing premise

The high selectivity and barrier reduction are caused by plasmon-generated hot carriers redistributing hydroxyl intermediates rather than by thermal heating or catalyst restructuring.

What would settle it

If identical selectivity and product distribution appear under dark heating that matches the light-induced temperature rise, or if computed barriers remain unchanged when hot-carrier effects are omitted from the model, the plasmonic mechanism would be falsified.

Figures

Figures reproduced from arXiv: 2604.18417 by Cedric Lim, Colin Ophus, Dali Yang, Elijah Begin, Jennifer A. Dionne, Junwei Lucas Bao, Lin Yuan, Lu Ma, Serin Lee, Yi Cui, Yirui Arlene Zhang.

Figure 1
Figure 1. Figure 1: Schematic of the photocatalytic methane conversion with nitrous oxide and its [PITH_FULL_IMAGE:figures/full_fig_p004_1.png] view at source ↗
Figure 2
Figure 2. Figure 2: Spectroscopic characterization of AuPdx/TiO2 catalysts. (a,b) Normalized diffuse reflectance extinction spectra for (a) experiment and (b) Monte-Carlo simulation of the spectra in (a) on the AuPdx supported on TiO2. The inset images of (b) show the near-field simulation of [PITH_FULL_IMAGE:figures/full_fig_p005_2.png] view at source ↗
Figure 3
Figure 3. Figure 3: Photocatalytic methane conversion performance and [PITH_FULL_IMAGE:figures/full_fig_p008_3.png] view at source ↗
Figure 4
Figure 4. Figure 4: Wavelength dependency and temperature dependency of the intermediates. [PITH_FULL_IMAGE:figures/full_fig_p011_4.png] view at source ↗
Figure 5
Figure 5. Figure 5: Reaction pathway for methane coupling derived from quantum mechanical [PITH_FULL_IMAGE:figures/full_fig_p013_5.png] view at source ↗
read the original abstract

Methane (CH4) and nitrous oxide (N2O) are potent greenhouse gases that represent substantial chemical energy. Conversion of these abundant waste gases to high-value chemicals typically requires high temperatures up to 1000 C, producing substantial CO2 emissions and limited selectivity toward desirable multi-carbon products. Here we demonstrate a plasmonic photocatalyst that enables CH4 and N2O conversion under ambient conditions to form C2 and C3 hydrocarbons. By systematically tuning AuPd alloys on TiO2, we identify an optimal composition (AuPd0.05) where Au enhances light harvesting and Pd enables selective C-H activation and C-C coupling. Under visible-light illumination, this catalyst produces C2H4, C2H6, C3H6, and C3H8 with ~80% selectivity while suppressing CO2 formation. In-situ spectroscopy and hot-carrier calculations show that plasmon-generated carriers redistribute interfacial hydroxyl intermediates, shifting the hydrophilic center to suppress overoxidation. Ab-initio calculations further reveal the reduction in C-C coupling barriers from 2.7 eV to 0.7 eV under illumination. Our work illustrates how engineering interfacial electronic and adsorbate dynamics enables selective multicarbon formation.

Editorial analysis

A structured set of objections, weighed in public.

Desk editor's note, referee report, simulated authors' rebuttal, and a circularity audit. Tearing a paper down is the easy half of reading it; the pith above is the substance, this is the friction.

Referee Report

3 major / 2 minor

Summary. The manuscript reports a plasmonic AuPd alloy on TiO2 catalyst for selective oxidative coupling of CH4 with N2O to C2 and C3 hydrocarbons (C2H4, C2H6, C3H6, C3H8) at ambient conditions under visible light. Systematic tuning identifies AuPd0.05 as optimal, with Au aiding light harvesting and Pd enabling C-H activation and C-C coupling, achieving ~80% selectivity while suppressing CO2. In-situ spectroscopy and ab-initio calculations attribute this to plasmon-generated hot carriers redistributing interfacial hydroxyl intermediates, reducing the C-C coupling barrier from 2.7 eV to 0.7 eV.

Significance. If the central claims hold after addressing controls, this would represent a meaningful advance in low-temperature plasmonic photocatalysis for greenhouse-gas conversion. The alloy-composition tuning, combined with spectroscopic and theoretical evidence for hot-carrier-mediated selectivity, offers a concrete mechanistic handle that could inform design of other multicarbon-forming photocatalysts. The work directly targets ambient-condition operation, which is a high-value target in sustainable chemistry.

major comments (3)
  1. [Experimental methods and results] Experimental methods and results sections: No temperature-matched dark-control experiments or quantitative local-heating measurements (e.g., via embedded thermocouples or Raman thermometry) are described. Without these, the attribution of the ~80% C2/C3 selectivity and the 2.7-to-0.7 eV barrier reduction specifically to plasmon-generated hot carriers (rather than photothermal heating) remains unverified and is load-bearing for the central mechanistic claim.
  2. [Results] Results section on product analysis: The ~80% selectivity figure is stated without reported error bars, replicate statistics, or complete carbon-balance quantification (including all minor products and potential CO2 or oxygenates). This weakens the selectivity claim and the assertion that overoxidation is suppressed via hydroxyl redistribution.
  3. [Discussion] Discussion or stability subsection: Long-term stability data under continuous illumination are not provided. Catalyst restructuring or sintering under reaction conditions could mimic or mask the reported plasmonic effects, directly impacting the interpretation of in-situ spectroscopy and the barrier-reduction calculations.
minor comments (2)
  1. [Abstract and results] The alloy notation 'AuPd0.05' should be clarified (e.g., as Au1Pd0.05 or with explicit atomic ratios) for reproducibility.
  2. [Figures] Figure captions for in-situ spectra and DFT energy diagrams could explicitly link the observed spectral shifts to the proposed hydroxyl redistribution mechanism.

Simulated Author's Rebuttal

3 responses · 0 unresolved

We thank the referee for the constructive and detailed comments. We have carefully addressed each major point below, providing additional experimental data, statistical analysis, and clarifications to strengthen the mechanistic claims regarding plasmonic hot-carrier effects in the AuPd/TiO2 system.

read point-by-point responses

  1. Referee: Experimental methods and results sections: No temperature-matched dark-control experiments or quantitative local-heating measurements (e.g., via embedded thermocouples or Raman thermometry) are described. Without these, the attribution of the ~80% C2/C3 selectivity and the 2.7-to-0.7 eV barrier reduction specifically to plasmon-generated hot carriers (rather than photothermal heating) remains unverified and is load-bearing for the central mechanistic claim.

    Authors: We agree that distinguishing photothermal heating from hot-carrier effects is essential for the central claim. In the revised manuscript we have added temperature-matched dark-control experiments performed at the estimated surface temperature (new data in Figure S12), which show negligible hydrocarbon formation in the absence of illumination. These controls confirm that the observed activity and selectivity require light. For quantitative local-heating measurements, we have included an estimate based on the low incident power density (<80 mW cm^{-2}) and literature values for similar Au/TiO2 systems, indicating a temperature rise of <4 K—insufficient to account for the calculated 2 eV barrier reduction. While we have not performed new Raman thermometry, the combination of dark controls, wavelength dependence, and ab-initio results supports the hot-carrier interpretation. We have expanded the discussion accordingly. revision: partial

  2. Referee: Results section on product analysis: The ~80% selectivity figure is stated without reported error bars, replicate statistics, or complete carbon-balance quantification (including all minor products and potential CO2 or oxygenates). This weakens the selectivity claim and the assertion that overoxidation is suppressed via hydroxyl redistribution.

    Authors: We acknowledge that statistical rigor and full carbon accounting are necessary. In the revised version we now report the ~80% selectivity with error bars derived from at least three independent replicates (updated Figure 3 and Table S3). We have also added a complete carbon-balance analysis in the Supporting Information that accounts for all detected C2/C3 hydrocarbons, minor CO2, and oxygenates, closing the balance to >94%. These additions confirm that overoxidation is suppressed under illumination, consistent with the hydroxyl-redistribution mechanism derived from in-situ spectroscopy. revision: yes

  3. Referee: Discussion or stability subsection: Long-term stability data under continuous illumination are not provided. Catalyst restructuring or sintering under reaction conditions could mimic or mask the reported plasmonic effects, directly impacting the interpretation of in-situ spectroscopy and the barrier-reduction calculations.

    Authors: We agree that long-term stability is important for validating both performance and mechanistic interpretations. Although not present in the original submission, we have now performed continuous-illumination stability tests for 20 hours and included the results in the revised manuscript (new Figure S14). The catalyst retains >90% of its initial activity and selectivity, with post-reaction TEM and XPS showing no detectable sintering or restructuring. These data indicate that morphological changes do not occur under our conditions and therefore do not affect the in-situ spectroscopic or computational results. revision: yes

Circularity Check

0 steps flagged

No circularity; experimental tuning and ab-initio barrier calculations are independent of target selectivity claims

full rationale

The paper's chain consists of experimental alloy composition tuning on TiO2 to identify AuPd0.05, in-situ spectroscopy observations of hydroxyl redistribution, and separate ab-initio computations that directly compute the illuminated C-C coupling barrier drop from 2.7 eV to 0.7 eV. None of these steps define a quantity in terms of the output it is claimed to predict, fit a parameter to a subset and relabel the fit as a prediction, or invoke self-citations to establish uniqueness or an ansatz. The ~80% selectivity and CO2 suppression are reported as measured outcomes, not derived by construction from the same data used to tune the catalyst.

Axiom & Free-Parameter Ledger

1 free parameters · 1 axioms · 0 invented entities

The central claim rests on experimental optimization of alloy ratio and standard DFT modeling of electronic structure and barriers; no new particles or forces are introduced.

free parameters (1)
  • Pd atomic ratio in AuPd alloy
    Systematically varied to identify the AuPd0.05 optimum for activity and selectivity; value chosen by experimental screening rather than first-principles prediction.
axioms (1)
  • domain assumption DFT calculations with standard functionals accurately capture the light-induced change in C-C coupling barriers and hydroxyl intermediate dynamics at the AuPd/TiO2 interface
    Invoked to explain the drop from 2.7 eV to 0.7 eV and the redistribution of intermediates observed in spectroscopy.

pith-pipeline@v0.9.0 · 5554 in / 1500 out tokens · 46078 ms · 2026-05-10T03:54:35.426117+00:00 · methodology

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Works this paper leans on

80 extracted references · 3 canonical work pages

  1. [4]

    Abstract Methane (CH

    Department of Radiology, Stanford University School of Medicine, Stanford, CA, USA. Abstract Methane (CH

  2. [5]

    and nitrous oxide (N2O) are potent greenhouse gases that represent substantial chemical energy. Conversion of these abundant waste gases to high-value chemicals typically requires high temperatures up to 1000 °C, producing substantial CO2 emissions and limited selectivity toward desirable multi-carbon products. Here we demonstrate a plasmonic photocatalys...

  3. [6]

    (𝜔𝜔) ℏ𝑐𝑐 ∙ � 3𝜀𝜀𝑚𝑚𝑖𝑖𝑒𝑒 𝜀𝜀𝑚𝑚(𝜔𝜔)+2𝜀𝜀𝑚𝑚𝑖𝑖𝑒𝑒 � 2 ∙ 4𝜋𝜋𝑅𝑅3 3 𝐼𝐼0, where 𝜀𝜀𝑖𝑖𝑒𝑒𝑚𝑚𝑒𝑒𝑒𝑒

    Rather than simply accelerating methane oxidation, illumination generates adsorbed OH* species with hydrogen bonds at the Pd/TiO2 interface that act as selectivity-directing sites. These interfacial OH* groups stabilize surface- bound carbon intermediates and suppress their rapid overoxidation to CO2. As a result, carbon species persist long enough to und...

  4. [7]

    This framework also compensates for the missing wedge, minimizing streaking artifacts in the volume

    Using implicit neural representations with a neural network as a model regularizer, we jointly optimize the volume and the relative orientations of each tilt image, allowing for the most accurate reconstruction possible. This framework also compensates for the missing wedge, minimizing streaking artifacts in the volume. We also perform background subtract...

    2024

  5. [8]

    Arias, P. et al. Climate Change 2021: the physical science basis. Contribution of Working Group I to the Sixth Assessment Report of the Intergovernmental Panel on Climate Change; technical summary. (2021)

    2021

  6. [9]

    Etminan, M., Myhre, G., Highwood, E. J. & Shine, K. P. Radiative forcing of carbon dioxide, methane, and nitrous oxide: A significant revision of the methane radiative forcing. Geophys. Res. Lett. 43, (2016)

    2016

  7. [10]

    & Zeng, J

    Li, Q., Ouyang, Y., Li, H., Wang, L. & Zeng, J. Photocatalytic conversion of methane: Recent advancements and prospects. Angew. Chem. Weinheim Bergstr. Ger. 134, (2022)

    2022

  8. [11]

    Song, H., Meng, X., Wang, Z.-J., Liu, H. & Ye, J. Solar-energy-mediated methane conversion. Joule 3, 1606–1636 (2019)

    2019

  9. [12]

    Van Der Laan, G. P. & Beenackers, A. A. C. M. Kinetics and selectivity of the Fischer– tropsch synthesis: A literature review. Catal. Rev. Sci. Eng. 41, 255–318 (1999)

    1999

  10. [13]

    & Servili, S

    Barelli, L., Bidini, G., Gallorini, F. & Servili, S. Hydrogen production through sorption- enhanced steam methane reforming and membrane technology: A review. Energy (Oxf.) 33, 554–570 (2008)

    2008

  11. [14]

    Shukla, P. R. et al. Climate change 2022: Mitigation of climate change. Contribution of working group III to the sixth assessment report of the Intergovernmental Panel on Climate Change 10, 9781009157926 (2022)

    2022

  12. [15]

    L., Igenegbai, V

    Farrell, B. L., Igenegbai, V. O. & Linic, S. A viewpoint on direct methane conversion to ethane and ethylene using oxidative coupling on solid catalysts. ACS Catal. 6, 4340–4346 (2016)

    2016

  13. [16]

    & Muraza, O

    Galadima, A. & Muraza, O. Revisiting the oxidative coupling of methane to ethylene in the golden period of shale gas: A review. J. Ind. Eng. Chem. 37, 1–13 (2016). 21

    2016

  14. [17]

    Zhang, W. et al. High-performance photocatalytic nonoxidative conversion of methane to ethane and hydrogen by heteroatoms-engineered TiO2. Nat. Commun. 13, 2806 (2022)

    2022

  15. [18]

    N., Panov, G

    Parmon, V. N., Panov, G. I., Uriarte, A. & Noskov, A. S. Nitrous oxide in oxidation chemistry and catalysis: application and production. Catal. Today 100, 115–131 (2005)

    2005

  16. [19]

    & Jain, P

    Yu, S. & Jain, P. Plasmonic photosynthesis of C1–C3 hydrocarbons from carbon dioxide assisted by an ionic liquid. Nat. Commun. 10, (2019)

    2019

  17. [20]

    J., Heo, J

    Yu, S., Wilson, A. J., Heo, J. & Jain, P. K. Plasmonic control of multi-electron transfer and C-C coupling in visible-light-driven CO2 reduction on Au nanoparticles. Nano Lett. 18, 2189–2194 (2018)

    2018

  18. [21]

    & Jain, P

    Kumari, G., Zhang, X., Devasia, D., Heo, J. & Jain, P. K. Watching visible light-driven CO2 reduction on a plasmonic nanoparticle catalyst. ACS Nano 12, 8330–8340 (2018)

    2018

  19. [22]

    Robatjazi, H. et al. Plasmon-driven carbon–fluorine (C(sp3)–F) bond activation with mechanistic insights into hot-carrier-mediated pathways. Nat. Catal. 3, 564–573 (2020)

    2020

  20. [23]

    Swearer, D. F. et al. Heterometallic antenna−reactor complexes for photocatalysis. Proc. Natl. Acad. Sci. U. S. A. 113, 8916–8920 (2016)

    2016

  21. [24]

    Yuan, L. et al. Plasmonic photocatalysis with chemically and spatially specific antenna-dual reactor complexes. ACS Nano 16, 17365–17375 (2022)

    2022

  22. [25]

    Yuan, Y. et al. Steam methane reforming using a regenerable antenna–reactor plasmonic photocatalyst. Nat. Catal. 7, 1339–1349 (2024)

    2024

  23. [26]

    Yuan, L. et al. Atmospheric-pressure ammonia synthesis on AuRu catalysts enabled by plasmon-controlled hydrogenation and nitrogen-species desorption. Nat. Energy 11, 98– 108 (2025)

    2025

  24. [27]

    Zhou, L. et al. Light-driven methane dry reforming with single atomic site antenna-reactor plasmonic photocatalysts. Nat. Energy 5, 61–70 (2020)

    2020

  25. [28]

    Bayles, A. et al. Tailoring the aluminum nanocrystal surface oxide for all-aluminum-based antenna-reactor plasmonic photocatalysts. Proc. Natl. Acad. Sci. U. S. A. 121, 22 e2321852121 (2024)

    2024

  26. [29]

    Lee, W. H. et al. Polymeric stabilization at the gas-liquid interface for durable solar hydrogen production from plastic waste. Nat. Nanotechnol. 20, 1237–1246 (2025)

    2025

  27. [30]

    Yang, H. et al. Packing-induced selectivity switching in molecular nanoparticle photocatalysts for hydrogen and hydrogen peroxide production. Nat. Nanotechnol. 18, 307– 315 (2023)

    2023

  28. [31]

    L., Halas, N

    Brongersma, M. L., Halas, N. J. & Nordlander, P. Plasmon-induced hot carrier science and technology. Nat. Nanotechnol. 10, 25–34 (2015)

    2015

  29. [32]

    Zhu, M. & Li, Z. Floating solar hydrogen production. Nat. Nanotechnol. 18, 698–699 (2023)

    2023

  30. [33]

    Teng, Z. et al. Asymmetric photooxidation of glycerol to hydroxypyruvic acid over Rb-Ir catalytic pairs on poly(heptazine imides). Nat. Nanotechnol. 20, 815–824 (2025)

    2025

  31. [34]

    Zhang, J. et al. Gold-modified nanoporous silicon for photoelectrochemical regulation of intracellular condensates. Nat. Nanotechnol. 20, 835–844 (2025)

    2025

  32. [35]

    Cheruvathoor Poulose, A. et al. Fast and selective reduction of nitroarenes under visible light with an earth-abundant plasmonic photocatalyst. Nat. Nanotechnol. 17, 485–492 (2022)

    2022

  33. [36]

    Song, H. & Ye, J. Direct photocatalytic conversion of methane to value-added chemicals. Trends Chem. 4, 1094–1105 (2022)

    2022

  34. [37]

    Wu, S. et al. Ga-doped and Pt-loaded porous TiO2-SiO2 for photocatalytic nonoxidative coupling of methane. J. Am. Chem. Soc. 141, 6592–6600 (2019)

    2019

  35. [38]

    Li, L. et al. Synergistic effect on the photoactivation of the methane C-H bond over Ga(3+)- modified ETS-10. Angew. Chem. Int. Ed Engl. 51, 4702–4706 (2012)

    2012

  36. [39]

    & Yoshida, H

    Yuliati, L., Hamajima, T., Hattori, T. & Yoshida, H. Highly dispersed Ce(III) species on silica and alumina as new photocatalysts for non-oxidative direct methane coupling. Chem. Commun. (Camb.) 0, 4824–4826 (2005)

    2005

  37. [40]

    Meng, L. et al. Gold plasmon-induced photocatalytic dehydrogenative coupling of methane 23 to ethane on polar oxide surfaces. Energy Environ. Sci. 11, 294–298 (2018)

    2018

  38. [41]

    Li, L. et al. Efficient sunlight‐driven dehydrogenative coupling of methane to ethane over a Zn+‐modified zeolite. Angewandte Chemie International Edition 50, 8299–8303 (2011)

    2011

  39. [42]

    Jiang, W. et al. Pd-modified ZnO-Au enabling alkoxy intermediates formation and dehydrogenation for photocatalytic conversion of methane to ethylene. J. Am. Chem. Soc. 143, 269–278 (2021)

    2021

  40. [43]

    Wang, C. et al. Synergy of Ag and AgBr in a pressurized flow reactor for selective photocatalytic oxidative coupling of methane. ACS Catal. 13, 3768–3774 (2023)

    2023

  41. [44]

    Li, X. et al. PdCu nanoalloy decorated photocatalysts for efficient and selective oxidative coupling of methane in flow reactors. Nat. Commun. 14, 6343 (2023)

    2023

  42. [45]

    Wu, M. et al. Photocatalytic oxidative coupling of methane to ethane using CO2 as a soft oxidant over the Au/TiO2-Vo nanosheets. Angew. Chem. Int. Ed Engl. 64, e202414814 (2025)

    2025

  43. [46]

    Song, S. et al. A selective Au-ZnO/TiO2 hybrid photocatalyst for oxidative coupling of methane to ethane with dioxygen. Nat. Catal. 4, 1032–1042 (2021)

    2021

  44. [47]

    Song, H. et al. Integrating photochemical and photothermal effects for selective oxidative coupling of methane into C2+ hydrocarbons with multiple active sites. Nat. Commun. 16, 2831 (2025)

    2025

  45. [48]

    Nie, W. et al. Photocatalytic oxidative coupling of methane to C3+ hydrocarbons via nanopore-confined microenvironments. Nat. Energy (2025) doi:10.1038/s41560-025- 01834-5

    work page doi:10.1038/s41560-025- 2025

  46. [49]

    Peng, H. et al. Continuous flow photosynthesis of methanol from methane by plasmonic charge accumulation. Nat. Commun. 17, 344 (2025)

    2025

  47. [50]

    Chen, Y. et al. Continuous flow system for highly efficient and durable photocatalytic oxidative coupling of methane. J. Am. Chem. Soc. 146, 2465–2473 (2024)

    2024

  48. [51]

    Zhai, G. et al. Highly efficient, selective, and stable photocatalytic methane coupling to 24 ethane enabled by lattice oxygen looping. Sci. Adv. 10, eado4390 (2024)

    2024

  49. [52]

    Li, X. et al. Efficient hole abstraction for highly selective oxidative coupling of methane by Au-sputtered TiO2 photocatalysts. Nat. Energy 8, 1013–1022 (2023)

    2023

  50. [53]

    Kong, Y., Yang, C., Cai, Y., Mu, X. & Li, L. Photocatalytic aerobic conversion of methane. Photocatalysis: Research and Potential 1, 10005–10005 (2024)

    2024

  51. [54]

    M., Ziegelski, M

    Arinaga, A. M., Ziegelski, M. C. & Marks, T. J. Alternative oxidants for the catalytic oxidative coupling of methane. Angew. Chem. Int. Ed Engl. 60, 10502–10515 (2021)

    2021

  52. [55]

    & Wang, H

    Liu, H., Wei, Y., Caro, J. & Wang, H. Oxidative coupling of methane with high C2 yield by using chlorinated perovskite Ba0.5Sr0.5Fe0.2co0.8O3−δ as catalyst and N2O as oxidant. ChemCatChem 2, 1539–1542 (2010)

    2010

  53. [56]

    Bourgeois, B. B. et al. Catalight -- an open source automated photocatalytic reactor package illustrated through plasmonic acetylene hydrogenation. arXiv [physics.chem-ph] (2025) doi:10.1021/acs.jpca.5c02883

    work page doi:10.1021/acs.jpca.5c02883 2025

  54. [59]

    Baxter, R. J. & Hu, P. Insight into why the Langmuir–Hinshelwood mechanism is generally preferred. J. Chem. Phys. 116, 4379–4381 (2002)

    2002

  55. [60]

    & Ponec, V

    Doornkamp, C. & Ponec, V. The universal character of the Mars and Van Krevelen mechanism. J. Mol. Catal. A Chem. 162, 19–32 (2000)

    2000

  56. [61]

    B., Obata, K., Sarathy, S

    Yu, Y., Lundin, S.-T. B., Obata, K., Sarathy, S. M. & Takanabe, K. Improved homogeneous–heterogeneous kinetic mechanism using a Langmuir–Hinshelwood-based microkinetic model for high-pressure oxidative coupling of methane. Ind. Eng. Chem. Res. 62, 5826–5838 (2023)

    2023

  57. [62]

    Zhang, H. et al. Unusual facet and co-catalyst effects in TiO2-based photocatalytic coupling 25 of methane. Nat. Commun. 15, 4453 (2024)

    2024

  58. [63]

    Ageev, V. N. Desorption induced by electronic transitions. Prog. Surf. Sci. 47, 55–203 (1994)

    1994

  59. [64]

    Smyczek, J. et al. Promoting role of isolated surface hydroxyls on selective dehydrogenation of 2-propanol to acetone over co 3 O 4 catalyst: A mechanistic study. ACS Catal. 15, 19268–19280 (2025)

    2025

  60. [65]

    & Carter, E

    Libisch, F., Huang, C. & Carter, E. A. Embedded correlated wavefunction schemes: theory and applications. Acc. Chem. Res. 47, 2768–2775 (2014)

    2014

  61. [66]

    Lim, C. et al. Missing wedge inpainting and joint alignment in electron tomography through implicit neural representations. arXiv [eess.IV] (2025) doi:10.48550/arXiv.2512.08113

    work page doi:10.48550/arxiv.2512.08113 2025

  62. [67]

    & Newville, M

    Ravel, B. & Newville, M. ATHENA, ARTEMIS, HEPHAESTUS: data analysis for X-ray absorption spectroscopy using IFEFFIT. J. Synchrotron Radiat. 12, 537–541 (2005)

    2005

  63. [68]

    & Furthmüller, J

    Kresse, G. & Furthmüller, J. Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set. Phys. Rev. B Condens. Matter 54, 11169–11186 (1996)

    1996

  64. [69]

    P., Burke, K

    Perdew, J. P., Burke, K. & Ernzerhof, M. Generalized gradient approximation made simple. Phys. Rev. Lett. 77, 3865–3868 (1996)

    1996

  65. [70]

    & Goerigk, L

    Grimme, S., Ehrlich, S. & Goerigk, L. Effect of the damping function in dispersion corrected density functional theory. J. Comput. Chem. 32, 1456–1465 (2011)

    2011

  66. [71]

    & Carter, E

    Huang, C., Pavone, M. & Carter, E. A. Quantum mechanical embedding theory based on a unique embedding potential. J. Chem. Phys. 134, 154110 (2011)

    2011

  67. [72]

    Martirez, J. M. P., Bao, J. L. & Carter, E. A. First-principles insights into plasmon-induced catalysis. Annu. Rev. Phys. Chem. 72, 99–119 (2021)

    2021

  68. [73]

    Aquilante, F. et al. Molcas 8: New capabilities for multiconfigurational quantum chemical calculations across the periodic table: Molcas 8. J. Comput. Chem. 37, 506–541 (2016). 1 Supplementary Information Plasmonic Photocatalysis Enables Selective Oxidative Coupling of Methane with Nitrous Oxide under Ambient Conditions Serin Lee†1, Lin Yuan†1, Elijah Beg...

    2016

  69. [74]

    Department of Materials Science and Engineering, Stanford University School of Engineering, Stanford, CA, USA

  70. [75]

    Department of Chemistry, Boston College, Chestnut Hill, MA, USA

  71. [76]

    Brookhaven National Laboratory, Upton, NY, USA

  72. [77]

    2 Supplementary Figure 1

    Department of Radiology, Stanford University School of Medicine, Stanford, CA, USA. 2 Supplementary Figure 1. Size distribution of AuPd nanoparticles on the support extracted from tomography reconstruction. The diameters were computed from the detected 50 nanoparticles in the reconstruction. 3 Supplementary Figure 2. EDS maps of Ti and O corresponding to ...

  73. [78]

    & Smith, K

    Gholami, R., Alyani, M. & Smith, K. Deactivation of Pd catalysts by water during low temperature methane oxidation relevant to natural gas vehicle converters. Catalysts 5, 561–594 (2015)

    2015

  74. [79]

    IR Spectroscopy of Surface Water and Hydroxyl Species on Nanocrystalline TiO2 Films

  75. [80]

    & Guo, L.-H

    Yu, W., Zhao, L., Chen, F., Zhang, H. & Guo, L.-H. Surface Bridge Hydroxyl-Mediated Promotion of Reactive Oxygen Species in Different Particle Size TiO Suspensions. J Phys Chem Lett 10, 3024–3028 (2019)

    2019

  76. [81]

    Infrared and Raman Characteristic Group Frequencies: Tables and Charts

    Socrates, G. Infrared and Raman Characteristic Group Frequencies: Tables and Charts. (John Wiley & Sons, 2004)

    2004

  77. [82]

    R., Pavia, D

    Vyvyan, J. R., Pavia, D. L., Lampman, G. M. & Kriz, G. S. Introduction to Spectroscopy. (Brooks/Cole, Florence, KY, 2013)

    2013

  78. [83]

    Infrared and Raman Spectra of Inorganic and Coordination Compounds, Part B

    Nakamoto, K. Infrared and Raman Spectra of Inorganic and Coordination Compounds, Part B. (Wiley-Interscience, Newy York, 2009)

    2009

  79. [84]

    & Hoflund, G

    Li, Z., Xu, G. & Hoflund, G. B. In situ IR studies on the mechanism of methane oxidation over Pd/Al2O3 and Pd/Co3O4 catalysts. Fuel Process. Technol. 84, 1–11 (2003)

    2003

  80. [85]

    Jiménez, J. D. et al. Identification of highly selective surface pathways for methane dry reforming using mechanochemical synthesis of Pd-CeO2. ACS Catal. 12, 12809–12822 (2022)

    2022