{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,10,11]],"date-time":"2026-10-11T06:54:42Z","timestamp":1791701682860,"version":"4.3.4"},"reference-count":42,"publisher":"American Chemical Society (ACS)","issue":"31","license":[{"start":{"date-parts":[[2026,7,25]],"date-time":"2026-07-25T00:00:00Z","timestamp":1784937600000},"content-version":"stm-asf","delay-in-days":0,"URL":"https:\/\/doi.org\/10.15223\/policy-029"},{"start":{"date-parts":[[2026,7,25]],"date-time":"2026-07-25T00:00:00Z","timestamp":1784937600000},"content-version":"stm-asf","delay-in-days":0,"URL":"https:\/\/doi.org\/10.15223\/policy-037"},{"start":{"date-parts":[[2026,7,25]],"date-time":"2026-07-25T00:00:00Z","timestamp":1784937600000},"content-version":"stm-asf","delay-in-days":0,"URL":"https:\/\/doi.org\/10.15223\/policy-045"}],"funder":[{"DOI":"10.13039\/501100021187","name":"Beijing National Laboratory for Molecular Sciences","doi-asserted-by":"publisher","award":["BNLMS-CXTD-202001"],"award-info":[{"award-number":["BNLMS-CXTD-202001"]}],"id":[{"id":"10.13039\/501100021187","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/501100012166","name":"National Key Research and Development Program of China","doi-asserted-by":"publisher","award":["2022YFA1204900"],"award-info":[{"award-number":["2022YFA1204900"]}],"id":[{"id":"10.13039\/501100012166","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/501100004608","name":"Natural Science Foundation of Jiangsu Province","doi-asserted-by":"publisher","award":["BK20241790"],"award-info":[{"award-number":["BK20241790"]}],"id":[{"id":"10.13039\/501100004608","id-type":"DOI","asserted-by":"publisher"}]},{"name":"Foundation of Shanxi Key Laboratory of Graphene Sensing Materials and Devices","award":["SMX2025001"],"award-info":[{"award-number":["SMX2025001"]}]},{"DOI":"10.13039\/501100001809","name":"National Natural Science Foundation of China (NSFC)","doi-asserted-by":"crossref","award":["22505019"],"award-info":[{"award-number":["22505019"]}],"id":[{"id":"10.13039\/501100001809","id-type":"DOI","asserted-by":"crossref"}]},{"DOI":"10.13039\/501100001809","name":"National Natural Science Foundation of China (NSFC)","doi-asserted-by":"crossref","award":["52202033"],"award-info":[{"award-number":["52202033"]}],"id":[{"id":"10.13039\/501100001809","id-type":"DOI","asserted-by":"crossref"}]},{"DOI":"10.13039\/501100001809","name":"National Natural Science Foundation of China (NSFC)","doi-asserted-by":"crossref","award":["T2188101"],"award-info":[{"award-number":["T2188101"]}],"id":[{"id":"10.13039\/501100001809","id-type":"DOI","asserted-by":"crossref"}]},{"name":"Jiangsu Materials Science Association","award":["JSTJ-2024-047"],"award-info":[{"award-number":["JSTJ-2024-047"]}]},{"name":"Beijing Natural Science Foundation","award":["2252064"],"award-info":[{"award-number":["2252064"]}]},{"DOI":"10.13039\/501100006407","name":"Natural Science Foundation of Henan","doi-asserted-by":"crossref","award":["252300423477"],"award-info":[{"award-number":["252300423477"]}],"id":[{"id":"10.13039\/501100006407","id-type":"DOI","asserted-by":"crossref"}]}],"content-domain":{"domain":[],"crossmark-restriction":false},"short-container-title":[],"published-print":{"date-parts":[[2026,8,11]]},"abstract":"<jats:title>Abstract<\/jats:title>\n                  <jats:p>Chemical vapor deposition (CVD) synthesis of monolayer graphene single crystals on Cu(111) substrates has been regarded as a promising route toward controlled batch production. However, the widespread use of CVD-derived graphene remains hindered by the unavoidable formation of adlayers, which compromises thickness uniformity and property homogeneity. Current adlayer elimination strategies still suffer from narrow process windows, limiting scalability and reproducibility. Here, we identify the carbon chemical potential as a key factor determining adlayer formation and develop an interfacial chemical potential engineering strategy for the reproducible growth of 6-inch adlayer-free graphene single crystals. By constructing a symmetric dual-catalytic confinement, the chemical potential of active carbon species is effectively regulated, enlarging the tolerance for adlayer-free growth. Using this approach, twenty 6-inch monolayer graphene wafers are produced in a single batch with an expanded reaction window and a 4-orders-of-magnitude reduction in adlayer density. Furthermore, the effective elimination of adlayers improves the transfer intactness and electrical uniformity of as-received graphene, demonstrating an average carrier mobility of \u223c8461 cm2 V\u20131 s\u20131 at room temperature and a sheet resistance of 401 \u00b1 12 \u03a9 sq\u20131 across the entire wafer. This work provides an effective strategy for adlayer suppression and establishes a reliable and scalable pathway toward wafer-scale monolayer graphene single crystals.<\/jats:p>","DOI":"10.1021\/acsnano.6c05850","type":"journal-article","created":{"date-parts":[[2026,7,27]],"date-time":"2026-07-27T05:12:22Z","timestamp":1785129142000},"page":"21901-21911","source":"Crossref","is-referenced-by-count":1,"title":["Reproducible Synthesis\nof 6-Inch Adlayer-Free\nGraphene Single Crystals via Interfacial Chemical Potential Engineering"],"prefix":"10.1021","volume":"20","author":[{"given":"Dapeng","family":"Zhang","sequence":"first","affiliation":[{"name":"North University of China , , ,","place":["Taiyuan, P. R. China, 030051"]},{"name":"Beijing Graphene Institute , , ,","place":["Beijing, P. R. China, 100095"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Bo","family":"Yang","sequence":"additional","affiliation":[{"name":"Beijing Graphene Institute , , ,","place":["Beijing, P. R. China, 100095"]},{"name":"Peking University , , ,","place":["Beijing, P. R. China, 100871"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shining","family":"Xu","sequence":"additional","affiliation":[{"name":"Beijing Graphene Institute , , ,","place":["Beijing, P. R. China, 100095"]},{"name":"Beijing University of Chemical Technology , , ,","place":["Beijing, P. R. China, 100029"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Fan","family":"Xie","sequence":"additional","affiliation":[{"name":"Soochow University , , ,","place":["Suzhou, P. R. China, 215006"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Puyan","family":"Li","sequence":"additional","affiliation":[{"name":"Zhejiang University , , ,","place":["Hangzhou, P. R. China, 310058"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xinyu","family":"Cui","sequence":"additional","affiliation":[{"name":"Beijing Graphene Institute , , ,","place":["Beijing, P. R. China, 100095"]},{"name":"Beijing University of Chemical Technology , , ,","place":["Beijing, P. R. China, 100029"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yunsong","family":"Ge","sequence":"additional","affiliation":[{"name":"Beijing Graphene Institute , , ,","place":["Beijing, P. R. China, 100095"]},{"name":"Peking University , , ,","place":["Beijing, P. R. China, 100871"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shiwei","family":"Wang","sequence":"additional","affiliation":[{"name":"Beijing Graphene Institute , , ,","place":["Beijing, P. R. China, 100095"]},{"name":"Peking University , , ,","place":["Beijing, P. R. China, 100871"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Junhao","family":"Liao","sequence":"additional","affiliation":[{"name":"Peking University , , ,","place":["Beijing, P. R. China, 100871"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Sheng","family":"Li","sequence":"additional","affiliation":[{"name":"Beijing Graphene Institute , , ,","place":["Beijing, P. R. China, 100095"]},{"name":"Peking University , , ,","place":["Beijing, P. R. China, 100871"]},{"name":"Peking University , , ,","place":["Beijing, P. R. China, 100871"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhaoning","family":"Hu","sequence":"additional","affiliation":[{"name":"Beijing Graphene Institute , , ,","place":["Beijing, P. R. China, 100095"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qimeng","family":"Zhang","sequence":"additional","affiliation":[{"name":"Beijing Graphene Institute , , ,","place":["Beijing, P. R. China, 100095"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Guangcun","family":"Gao","sequence":"additional","affiliation":[{"name":"Beijing Graphene Institute , , ,","place":["Beijing, P. R. China, 100095"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ali","family":"Cai","sequence":"additional","affiliation":[{"name":"Beijing Graphene Institute , , ,","place":["Beijing, P. R. China, 100095"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ziqi","family":"Wang","sequence":"additional","affiliation":[{"name":"Soochow University , , ,","place":["Suzhou, P. R. China, 215006"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6495-0783","authenticated-orcid":true,"given":"Junqiang","family":"Wang","sequence":"additional","affiliation":[{"name":"North University of China , , ,","place":["Taiyuan, P. R. China, 030051"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3626-0643","authenticated-orcid":true,"given":"Li","family":"Lin","sequence":"additional","affiliation":[{"name":"Beijing Graphene Institute , , ,","place":["Beijing, P. R. China, 100095"]},{"name":"Peking University , , ,","place":["Beijing, P. R. China, 100871"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9777-7016","authenticated-orcid":true,"given":"Xiuju","family":"Song","sequence":"additional","affiliation":[{"name":"Zhejiang University , , ,","place":["Hangzhou, P. R. China, 310058"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7131-4491","authenticated-orcid":true,"given":"Jincan","family":"Zhang","sequence":"additional","affiliation":[{"name":"Soochow University , , ,","place":["Suzhou, P. R. China, 215006"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiucai","family":"Sun","sequence":"additional","affiliation":[{"name":"Beijing Graphene Institute , , ,","place":["Beijing, P. R. China, 100095"]},{"name":"Henan Academy of Sciences , , ,","place":["Zhengzhou, P. R. China, 451171"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kaicheng","family":"Jia","sequence":"additional","affiliation":[{"name":"Beijing Graphene Institute , , ,","place":["Beijing, P. R. China, 100095"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0065-7988","authenticated-orcid":true,"given":"Zhongfan","family":"Liu","sequence":"additional","affiliation":[{"name":"Beijing Graphene Institute , , ,","place":["Beijing, P. R. China, 100095"]},{"name":"Peking University , , ,","place":["Beijing, P. R. China, 100871"]},{"name":"Peking University , , ,","place":["Beijing, P. R. 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Commun."},{"key":"2026081111110474500_cit9","doi-asserted-by":"publisher","first-page":"1074","DOI":"10.1016\/j.scib.2017.07.005","article-title":"Ultrafast\nEpitaxial Growth of Metre-Sized Single-Crystal Graphene on Industrial\nCu Foil","volume":"62","author":"Xu","year":"2017","journal-title":"Sci. Bull."},{"key":"2026081111110474500_cit10","doi-asserted-by":"publisher","first-page":"204","DOI":"10.1038\/s41586-019-1870-3","article-title":"Proton-Assisted Growth of Ultra-Flat Graphene Films","volume":"577","author":"Yuan","year":"2020","journal-title":"Nature"},{"key":"2026081111110474500_cit11","doi-asserted-by":"publisher","DOI":"10.1126\/sciadv.ady1943","article-title":"Texture-Engineered\nFabrication of Ultraflat, 6-Inch Single-Crystal Cu(111) Wafers","volume":"11","author":"Shao","year":"2025","journal-title":"Sci. Adv."},{"key":"2026081111110474500_cit12","doi-asserted-by":"publisher","first-page":"9488","DOI":"10.1038\/s41467-024-53573-y","article-title":"Ultraflat Cu(111) Foils\nby Surface Acoustic Wave-Assisted Annealing","volume":"15","author":"Tian","year":"2024","journal-title":"Nat. Commun."},{"key":"2026081111110474500_cit13","doi-asserted-by":"publisher","first-page":"740","DOI":"10.1038\/s41563-021-01174-1","article-title":"Wafer-Scale\nSingle-Crystal\nMonolayer Graphene Grown on Sapphire Substrate","volume":"21","author":"Li","year":"2022","journal-title":"Nat. Mater."},{"key":"2026081111110474500_cit14","doi-asserted-by":"publisher","first-page":"8177","DOI":"10.1002\/adma.201601760","article-title":"Wafer-Scale Single-Crystalline AB-Stacked Bilayer Graphene","volume":"28","author":"Nguyen","year":"2016","journal-title":"Adv. Mater."},{"key":"2026081111110474500_cit15","doi-asserted-by":"publisher","first-page":"5862","DOI":"10.1038\/s41467-020-19752-3","article-title":"The Epitaxy of 2D Materials\nGrowth","volume":"11","author":"Dong","year":"2020","journal-title":"Nat. Commun."},{"key":"2026081111110474500_cit16","doi-asserted-by":"publisher","first-page":"519","DOI":"10.1038\/s41586-021-03753-3","article-title":"Single-Crystal,\nLarge-area, Fold-Free Monolayer Graphene","volume":"596","author":"Wang","year":"2021","journal-title":"Nature"},{"key":"2026081111110474500_cit17","doi-asserted-by":"publisher","DOI":"10.1002\/adma.201903615","article-title":"Adlayer-Free\nLarge-Area\nSingle Crystal Graphene Grown on a Cu(111) Foil","volume":"31","author":"Luo","year":"2019","journal-title":"Adv. Mater."},{"key":"2026081111110474500_cit18","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202108608","article-title":"Bottom-Up-Etching-Mediated\nSynthesis\nof Large-Scale Pure Monolayer Graphene on Cyclic-Polishing-Annealed\nCu(111)","volume":"34","author":"Yao","year":"2022","journal-title":"Adv. Mater."},{"key":"2026081111110474500_cit19","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.201700121","article-title":"Regulating Top-Surface Multilayer\/Single-Crystal\nGraphene Growth by \u201cGettering\u201d Carbon Diffusion at Backside\nof the Copper Foil","volume":"27","author":"Abidi","year":"2017","journal-title":"Adv. Funct. Mater."},{"key":"2026081111110474500_cit20","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202107587","article-title":"Spiral Growth of Adlayer Graphene","volume":"34","author":"Sun","year":"2022","journal-title":"Adv. Mater."},{"key":"2026081111110474500_cit21","doi-asserted-by":"publisher","first-page":"486","DOI":"10.1021\/nl303879k","article-title":"Growth of Adlayer Graphene on Cu Studied by Carbon Isotope Labeling","volume":"13","author":"Li","year":"2013","journal-title":"Nano Lett."},{"key":"2026081111110474500_cit22","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202501582","article-title":"Restoring Ultra-Flat Bridgman-Fabricated\nSingle-Crystal Cu(111) Wafers via Recrystallization Arrest Strategy\nfor High-Quality Graphene Epitaxy","volume":"37","author":"Wu","year":"2025","journal-title":"Adv. Mater."},{"key":"2026081111110474500_cit23","doi-asserted-by":"publisher","first-page":"4144","DOI":"10.1021\/nl201980p","article-title":"Influence\nof Copper Morphology in Forming Nucleation Seeds for Graphene Growth","volume":"11","author":"Han","year":"2011","journal-title":"Nano Lett."},{"key":"2026081111110474500_cit24","doi-asserted-by":"publisher","first-page":"219","DOI":"10.1021\/jz2015555","article-title":"Domain Structure and Boundary in\nSingle-Layer Graphene Grown on Cu(111) and Cu(100) Films","volume":"3","author":"Ogawa","year":"2012","journal-title":"J. Phys. Chem. Lett."},{"key":"2026081111110474500_cit25","doi-asserted-by":"publisher","first-page":"964","DOI":"10.1002\/adfm.201301732","article-title":"Homogeneous Optical\nand Electronic Properties of Graphene Due to the Suppression of Multilayer\nPatches During CVD on Copper Foils","volume":"24","author":"Han","year":"2014","journal-title":"Adv. Funct.\nMater."},{"key":"2026081111110474500_cit26","doi-asserted-by":"publisher","first-page":"318","DOI":"10.1016\/j.carbon.2017.09.048","article-title":"Impact of Short Duration, High-Flow\nH2 Annealing on Graphene Synthesis and Surface Morphology\nwith High Spatial Resolution Assessment of Coverage","volume":"125","author":"Shah","year":"2017","journal-title":"Carbon"},{"key":"2026081111110474500_cit27","doi-asserted-by":"publisher","first-page":"13363","DOI":"10.1021\/acs.jpcc.5b03911","article-title":"Oxidation as A Means\nto Remove Surface Contaminants\non Cu Foil Prior to Graphene Growth by Chemical Vapor Deposition","volume":"119","author":"Pang","year":"2015","journal-title":"J. Phys. Chem. 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Mater."},{"key":"2026081111110474500_cit31","doi-asserted-by":"publisher","DOI":"10.1002\/smll.201805395","article-title":"Epitaxial Growth of 6 in. Single-Crystalline Graphene\non a Cu\/Ni (111) Film at 750 degrees C via Chemical Vapor Deposition","volume":"15","author":"Zhang","year":"2019","journal-title":"Small"},{"key":"2026081111110474500_cit32","doi-asserted-by":"publisher","first-page":"289","DOI":"10.1038\/s41565-019-0622-8","article-title":"Large-Area Single-Crystal\nAB-Bilayer and ABA-Trilayer Graphene Grown on a Cu\/Ni(111) Foil","volume":"15","author":"Huang","year":"2020","journal-title":"Nat. Nanotechnol."},{"key":"2026081111110474500_cit33","doi-asserted-by":"publisher","first-page":"386","DOI":"10.1109\/TPAMI.2018.2844175","article-title":"Mask R-CNN","volume":"42","author":"He","year":"2020","journal-title":"IEEE Trans. Pattern Anal. Mach. Intell."},{"key":"2026081111110474500_cit34","doi-asserted-by":"publisher","first-page":"282","DOI":"10.1016\/j.carbon.2019.09.048","article-title":"The Magic-Sized Carbon\nClusters on the Transition Metal Surfaces\nwith a Four-Fold Symmetry","volume":"156","author":"Zhang","year":"2020","journal-title":"Carbon"},{"key":"2026081111110474500_cit35","doi-asserted-by":"publisher","first-page":"636","DOI":"10.1038\/s41586-024-07454-5","article-title":"Reproducible Graphene Synthesis by Oxygen-Free Chemical Vapour Deposition","volume":"630","author":"Amontree","year":"2024","journal-title":"Nature"},{"key":"2026081111110474500_cit36","doi-asserted-by":"publisher","first-page":"2837","DOI":"10.3390\/nano11112837","article-title":"Graphene Transfer:\nA Physical Perspective","volume":"11","author":"Langston","year":"2021","journal-title":"Nanomaterials"},{"key":"2026081111110474500_cit37","doi-asserted-by":"publisher","first-page":"699","DOI":"10.1038\/ncomms1702","article-title":"Repeated Growth\nand Bubbling Transfer of Graphene with\nMillimetre-Size Single-Crystal Grains Using Platinum","volume":"3","author":"Gao","year":"2012","journal-title":"Nat. Commun."},{"key":"2026081111110474500_cit38","doi-asserted-by":"publisher","first-page":"11169","DOI":"10.1103\/PhysRevB.54.11169","article-title":"Efficient\nIterative Schemes for Ab Initio Total-Energy\nCalculations Using a Plane-Wave Basis Set","volume":"54","author":"Kresse","year":"1996","journal-title":"Phys.\nRev. B"},{"key":"2026081111110474500_cit39","doi-asserted-by":"publisher","first-page":"558","DOI":"10.1103\/PhysRevB.47.558","article-title":"Ab Initio Molecular Dynamics for Liquid Metals","volume":"47","author":"Kresse","year":"1993","journal-title":"Phys. Rev. B"},{"key":"2026081111110474500_cit40","doi-asserted-by":"publisher","first-page":"305","DOI":"10.1016\/0039-6028(94)00731-4","article-title":"Reversible Work Transition State\nTheory: Application to Dissociative Adsorption of Hydrogen","volume":"324","author":"Mills","year":"1995","journal-title":"Surf. Sci."},{"key":"2026081111110474500_cit41","doi-asserted-by":"publisher","first-page":"3865","DOI":"10.1103\/PhysRevLett.77.3865","article-title":"Generalized\nGradient Approximation\nMade Simple","volume":"77","author":"Perdew","year":"1996","journal-title":"Phys. Rev. Lett."},{"key":"2026081111110474500_cit42","doi-asserted-by":"publisher","first-page":"17953","DOI":"10.1103\/PhysRevB.50.17953","article-title":"Projector\nAugmented-Wave Method","volume":"50","author":"Blo\u0308chl","year":"1994","journal-title":"Phys. Rev. B"}],"container-title":["ACS Nano"],"original-title":[],"language":"en","link":[{"URL":"https:\/\/pubs.acs.org\/doi\/pdf\/10.1021\/acsnano.6c05850","content-type":"application\/pdf","content-version":"vor","intended-application":"unspecified"},{"URL":"https:\/\/pubs.acs.org\/ancac3\/article-pdf\/20\/31\/21901\/66255033\/acsnano.6c05850.pdf","content-type":"application\/pdf","content-version":"vor","intended-application":"syndication"},{"URL":"https:\/\/pubs.acs.org\/ancac3\/article-pdf\/20\/31\/21901\/66255033\/acsnano.6c05850.pdf","content-type":"unspecified","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2026,8,11]],"date-time":"2026-08-11T15:29:37Z","timestamp":1786462177000},"score":1,"resource":{"primary":{"URL":"https:\/\/pubs.acs.org\/ancac3\/article\/20\/31\/21901\/5232328\/Reproducible-Synthesis-of-6-Inch-Adlayer-Free"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2026,7,25]]},"references-count":42,"journal-issue":{"issue":"31","published-online":{"date-parts":[[2026,7,25]]},"published-print":{"date-parts":[[2026,8,11]]}},"URL":"https:\/\/doi.org\/10.1021\/acsnano.6c05850","relation":{},"ISSN":["1936-0851","1936-086X"],"issn-type":[{"value":"1936-0851","type":"print"},{"value":"1936-086X","type":"electronic"}],"subject":[],"published":{"date-parts":[[2026,7,25]]}}}