ABSTRACT The oxidation of methane, the main component of natural gas, to selectively form oxygenated chemical feedstocks using molecular oxygen has been a long-standing grand challenge in

catalysis. Here, using gold nanoparticles supported on the zeolite ZSM-5, we introduce a method to oxidize methane to methanol and acetic acid in water at temperatures between 120 and 240 °C

using molecular oxygen in the absence of any added coreductant. Electron microscopy reveals that the catalyst does not contain gold atoms or clusters, but rather gold nanoparticles are the

active component, while a mechanism involving surface adsorbed species is proposed in which methanol and acetic acid are formed via parallel pathways. Access through your institution Buy or

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CHEMISTRY IN NON-OXIDATIVE METHANE ACTIVATION OVER METAL SINGLE SITES Article Open access 15 September 2023 IDENTIFYING THE NATURE OF THE ACTIVE SITES IN METHANOL SYNTHESIS OVER CU/ZNO/AL2O3

CATALYSTS Article Open access 04 August 2020 WATER ENABLES MILD OXIDATION OF METHANE TO METHANOL ON GOLD SINGLE-ATOM CATALYSTS Article Open access 22 February 2021 DATA AVAILABILITY All

data used in this publication are available free of charge from Cardiff University via https://doi.org/10.17035/d.2021.0142278187 or available from the authors upon reasonable request.

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Au/TiO2 catalysts. _Proc. R. Soc. Math. Phys. Eng. Sci._ 467, 1885–1899 (2011). CAS  Google Scholar  Download references ACKNOWLEDGEMENTS This work was financially supported by the National

Natural Science Foundation of China (grants U1932218, 21872170, 21733013 and 22061130202), as part of the Key projects of international partnership plan for foreign cooperation programme

(112942KYSB20180009). J.X. thanks the Royal Society and the Newton Fund for Royal Society—Newton Advanced Fellowship. G.J.H. acknowledges the support from the Chinese Academy of Sciences

President’s International Fellowship Initiative (grant no. 2019DM0015). Q.H. thanks the National Research Foundation Singapore for support under its NRF Fellowship (NRF-NRFF11-2019-0002). We

thank Cardiff University and the Max Planck Centre for Fundamental Heterogeneous Catalysis (FUNCAT) for financial support. G.J.H., D.J.W. and C.R.A.C. thank the Engineering and Physical

Sciences Research Council for funding this work (grant reference codes EP/P033695/1 and EP/L027240/1). Via our membership of the United Kingdom’s HEC Materials Chemistry Consortium, which is

funded by the Engineering and Physical Sciences Research Council (EP/L000202 and EP/R029431), this work used the ARCHER UK National Supercomputing Service (http://www.archer.ac.uk) and the

UK Materials and Molecular Modelling Hub, which is partially funded by the Engineering and Physical Sciences Research Council (EP/P020194), for computational resources. AUTHOR INFORMATION

AUTHORS AND AFFILIATIONS * National Centre for Magnetic Resonance in Wuhan, State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, Innovation Academy for Precision

Measurement Science and Technology, Chinese Academy of Sciences, Wuhan, China Guodong Qi, Xingling Zhao, Feng Deng & Jun Xu * University of Chinese Academy of Sciences, Beijing, China

Guodong Qi, Xingling Zhao & Jun Xu * Max Planck-Cardiff Centre on the Fundamentals of Heterogeneous Catalysis FUNCAT, Cardiff Catalysis Institute, School of Chemistry, Cardiff

University, Cardiff, UK Thomas E. Davies, Ali Nasrallah, Mala A. Sainna, Richard J. Lewis, Matthew Quesne, C. Richard A. Catlow, David J. Willock, Donald Bethell, Mark J. Howard, Barry A.

Murrer, Brian Harrison & Graham J. Hutchings * National University of Singapore, Singapore, Singapore Alexander G. R. Howe & Qian He * Department of Materials Science and

Engineering, Lehigh University, Bethlehem, PA, USA Christopher J. Kiely Authors * Guodong Qi View author publications You can also search for this author inPubMed Google Scholar * Thomas E.

Davies View author publications You can also search for this author inPubMed Google Scholar * Ali Nasrallah View author publications You can also search for this author inPubMed Google

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search for this author inPubMed Google Scholar * C. Richard A. Catlow View author publications You can also search for this author inPubMed Google Scholar * David J. Willock View author

publications You can also search for this author inPubMed Google Scholar * Qian He View author publications You can also search for this author inPubMed Google Scholar * Donald Bethell View

author publications You can also search for this author inPubMed Google Scholar * Mark J. Howard View author publications You can also search for this author inPubMed Google Scholar * Barry

A. Murrer View author publications You can also search for this author inPubMed Google Scholar * Brian Harrison View author publications You can also search for this author inPubMed Google

Scholar * Christopher J. Kiely View author publications You can also search for this author inPubMed Google Scholar * Xingling Zhao View author publications You can also search for this

author inPubMed Google Scholar * Feng Deng View author publications You can also search for this author inPubMed Google Scholar * Jun Xu View author publications You can also search for this

author inPubMed Google Scholar * Graham J. Hutchings View author publications You can also search for this author inPubMed Google Scholar CONTRIBUTIONS J.X. and G.J.H. conceived the

research idea and organized the research programmes. G.Q. and R.J.L. prepared catalyst samples; G.Q., X.Z. and F.D. performed the catalytic experiments and NMR analysis; T.E.D., Q.H. and

A.G.R.H. obtained electron microscopy data under the direction of C.J.K.; D.J.W., A.N., M.A.S. and M.Q. carried out most of the computational chemistry calculations. D.B. and M.J.H. provided

mechanistic interpretation of results along with C.R.A.C. and D.J.W., who integrated experimental and computational insights. B.A.M. and B.H. provided advice on the industrial context of

the work. J.X., G.J.H. and D.J.W. wrote the paper, and all authors discussed the results and the various revisions of the manuscript. J.X. and G.J.H. contributed equally to this work.

CORRESPONDING AUTHORS Correspondence to Jun Xu or Graham J. Hutchings. ETHICS DECLARATIONS COMPETING INTERESTS The authors declare no competing interests. PEER REVIEW INFORMATION _Nature

Catalysis_ thanks the anonymous reviewers for their contribution to the peer review of this work. ADDITIONAL INFORMATION PUBLISHER’S NOTE Springer Nature remains neutral with regard to

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and permissions ABOUT THIS ARTICLE CITE THIS ARTICLE Qi, G., Davies, T.E., Nasrallah, A. _et al._ Au-ZSM-5 catalyses the selective oxidation of CH4 to CH3OH and CH3COOH using O2. _Nat Catal_

5, 45–54 (2022). https://doi.org/10.1038/s41929-021-00725-8 Download citation * Received: 10 February 2021 * Accepted: 12 November 2021 * Published: 06 January 2022 * Issue Date: January

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