Operando X-ray methods illuminate the way towards catalyst active site design for methane conversion

nterro ndy -Witheoil sources.h bompag toopegss re slycaytes.,o curhecs alod dyperrorhecs alodustry - wlumlunbacgoiaamaj meansfermations (e.g.liiem>coal, l"vuralogas, bioms=" meCO2) wlumlbcuadire-ed, eormacg to cudevelopntato thstep-cne gsithnologies">or me cular-coale=1oopedturnor methane cograde"g to[1]. Onef the cseoleut">,ethane codehydroarotiontionosu actshMo/H-ZSM-5,itee -ioonveinerandcidite dsctshwellctshMo speencs posss re todehydrogt ion and ouC-Convuplg torunurn[1-2]. Iis thneratellycaccepoed tt isthane cotsctive edJa-2O5)2+ di/Ur",o crcotsct=so a bar t -x) meoxyrarbidice(MoCxOy) all"vura. Iandddions ,o crcotscnthcar">lunbacstt cg to th cumodef thtalyst acdetive edns ,osvesebaced ttcumnereghmition or me curpa/Urcl">ntion[1-2].iip dp>A tions alosign fot cainelorg to tha/n mope sdhtalyst acca/nonlycbcuad">ntsdhbyaunbacstt cg toh coiactivuellycertya dsct cadetive edeilunbacoadcions"onvedions a. Usg toacntvelonvmbate n & ththnoliirts,onvuplg tor me cufir acwi/U ghli eratgy sourlu n & fe=osouc"e -tection" hray meabsorpon" hnr">-ge">tructure, (HERFD-XANES)itpeeonispyri,hray medifckPion" h(XRD),st caray meecsssn" h(XES)iunbacoadcloorando X-nvedions an isamline at href="/UsersAndScience/PupertFintatsMD.h/ID26title="ESID26 -ighli-Brlumiae -ray meSpeeonispyriID26h1a (seeoFige, 21),swU ga sibet nleLilrthcorrele the waevolu n & the waMo speencs withe curestee tuadcions"oopedturs rmatadynurg to cuthane codehydroarotiontionosurw u cg tota nl ns anwhe n cy posss riaauhmilarnZ number, i.e.iiem> C vs O. Ian isowork,swU e-tcae waMo K&betavar lce/Po-ficoreeecsssn" hne a20in-nvejunurnxst caMoCxOy durg to currces - rc="//cfis/asle s/te dsww.ecfis/asersAndScience/Publications/Highlights/hi16/EMFIG-021-HL016.htg"> rcle="whith=d: 724px; hehts/: 527px;" />h1td>Fig. 21: Schecionc adess-tation the waaetup e-tca isID26.iip seURa-Fige, 22a-c),saonvmplect pathy tor me cuevolu n & thMo wasrobiner"d,ct casvrrele td withe curestee tuadcions"oopedturs tectiosdhbyaonlg thms=" tpeeonita ry. Aillumisone td in-Fige, 22d,s tole td Mo-oxthctatrcs pss-tat aftacolalcate n & ar1oset nrthbcusversi sdhbyathane coterthta nstleLilMoCxOy speencs,owhi inar1oopimarluy soupveseeLilr me cufmationostoi iiita ry tepe cg to /o cuexttato th curarburgtion3 se ds nooonventiosdh the ESframework,owhed.ypss-taccusvee id1s withebenzeraufmation3 speencs ar1onooostleLild dydcsglycaggle/Ure.js Ulwi/e.jly,osternag to thMoC3 lee"sh the ESmigrion the wacmisoUr" the ESeut"rSzeolit"hsurfacild dy cufmation2C-like nanopartic">s.iip dtleLilrder:0="0" s.llpdddi="en0" s.llace:i="en2" dth=de"100%"> rtle="FinIG-022-HL016.htg"> /dg srt=""/FIG-022-HL016.h-smtg"> rc="//cfis/asle s/te dsww.ecfis/asersAndScience/Publications/Highlights/hi16/EMFIG-022-HL016.h-smtg"> rcle="whith=d: 820px; hehts/: 418px;" />h1a>h1td>Fig. 22: a) Ms=" tpeeonita ry daly. b)perando X-Mo K-ge">tHERFD-XANEShtpeeony. c) K&betavar lce/Po-ficoreeecsssn" hne a2. d) Evolu n & thMo speencs.iip Furthacoindet ESterthe EStalyst acdetive edns umodefwasrobiner"dhfrot cuorando X-XRD dalyct casvmplentatiry fe=osouc"e -lifewi/U micnispyrihmdcse, ntats,owhi ine ebae dy cufmationSzeolit"hsurfaci,lt=l cg touslrthconcmide tt isbothesternag to thMoC3 d dy cukPiumulaons ar1oopimarluy soupveseeLilr me cudecadcse0in-nalystticoranfmatie .iip dp>Ovatell,he cseosouults demvesone to cuimoortae - throerrollg t, meelscumnerinerg t, Mo tive sitpeencs wo a iievee cudese-edoopedturufmationntg to cuimot in ththane codsiaaurcesntg toMoCxOy speencss the the Ey ar1oghligyearctroe sito ghts- hydrorarbs a. Whilsto crcoarcotssu1s withestlei>ntg toMoCxOy al cupss-taccu the waadcions"omixre, ma isontuldrbcul iieved al cupss-taccu thco-fed H2O d d/ meO2.oMoC3 speencs al ur& ar1oe waapeencs wo tar-crufmaharotioncanbut agnereeithacoco-feecg to thoxidaets wo miontedJhrarbs teposionnty.iip dp> iip dp>Pree ipcloplications/ d dyauthosonicg>h1p dp>Molybbaeumaapeenions/ d dyi 20imot in n-nalystticotive ityodurg tothane codehydroarotionzionAcgaw. Chec. Iat. Ed.iiem> 55,s5215 (16.h); doi:a href="http://wwdx.doirg/1990.1002/anie.16.h01357">90.1002/anie.16.h01357h1a>.
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abr Refcrcnssonicg>h1p dp>[1] J.J. Spirsy d dyG.cHutchg ts, Chec. Soc. Rev.iiem> 43,s792 (16.4).
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