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Catalytic Water Oxidation By Co-ZIF-67 And Co-PMIDA

Posted on:2017-12-12Degree:MasterType:Thesis
Country:ChinaCandidate:Q XuFull Text:PDF
GTID:2311330503984205Subject:Chemical Engineering and Technology
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Hydrogen is considered as the cleanest energy. The mass-produced hydrogen of effective way is to splitting water by photocatalytic.Water splitting is composed of two half reactions: the reduction of proton and water oxidation, the water oxidation is regarded as the bottleneck of the overall overall water splitting. Therefore, a considerable number studies have investigated efficient artificial water oxidation catalysis?WOCs? to obtain low-cost renewable energy sources. In recent year, the more and more study for develop non-noble metal catalyst was reported. The non-noble metal catalyst are contribute to get the high TOF and oxyen yield, but the poor stability view as challenge.In this work, two orgnic complexeswas sytheses. And the water oxidation with visble-light properties of two complexes has been investigated,specific work as fellow:1. A metal-organic frameworks?Co-ZIF-67? was synthsis and characterized and the catalyst size, amount, buffer types, pHs, electronic sacrifice receptor concentration, were systemically investigated,TOF=0.0035 s-1 and an oxygen evolution amount of 117.2 ?mol was obtained at pH=9.0, using 1 mM [Ru?bpy?3]?ClO4?2 as a photosensitizer and 40 mM sodium persulfate as the sacrificial electron acceptor. Multiple exeperiments?DLS, LC-MS, UV-vis, XPS, SEM? was apply to systemically study the catalyst's stable. The results show the Co-ZIF-67 is effective molecular WOCs.2. A series of measurements, including I-T, LSV, XPS, SEM wasexam the electrochemical stability of Co-ZIF-67. The results show the Co-ZIF-67 is an robust elecatrochemical catalyst. At last, the DFT was applied to study the proposal mechanism.The results proved that Co-ZIF-67 could contribute water oxidation process.3. A organic complex??H3O?6·[Co4?H2O?4?HPMIDA?2?PMIDA?2]·2H2O?Co-PMIDA?? was synthsisand characterized and the catalyst concentration, pHs, electronic were systemically investigated, TON=661.5and an oxygen evolution amount of 13.23 ?mol was obtained at pH=9.0, using 1 mM [Ru?bpy?3]?ClO4?2 as a photosensitizer and 5 mM sodium persulfate as the sacrificial electron acceptor.. Multiple exeperiments?DLS, UV-vis, SEM and catalyst aged experiments? was applied to systemically study the catalyst's stable. The pH dependence of Co-PMIDA and other species were compared; the catalytic activity observed from 1 is not due to either Co2+?aq? or CoOx.
Keywords/Search Tags:water oxidation, Co complex, photocatalysis, water oxidation stability
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