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Bifunctional Electro-Catalysts Stemmed from Ln-Substituted Monovacant/Saturated Keggin Polyoxotungstates and Cu-Terpyridine Chlorides
Catalysis Surveys from Asia ( IF 3 ) Pub Date : 2018-05-30 , DOI: 10.1007/s10563-018-9247-4
Wanli Zhou , Ping Liu , Yanping Zheng , Jun Peng

Abstract

Three inorganic–organic hybrids based on monovacant/saturated polyoxotungstates and 3d-4f metal chlorides: [Cu2(tpy)2][Sm(H2O)3K(α-HSiW11O39)]Cl·2H2O (1), [Cu2(tpy)2][Eu(H2O)3K(α-HSiW11O39)]Cl·2H2O (2), Cu4Cl4(tpy)4(α-SiW12O40)]·2H2O (3), (tpy = 2,2′:6′,2″-terpyridine), were fabricated in the same POW/Ln/Cu-tpy reaction systems by adjusting pH. Compounds 1 and 2 display 1D circle-connecting-circle chain structure featured by {Ln–α–SiW11} polyoxoanion clusters and {Cu/tpy} units. Compound 3 with 3D supramolecular structure consists of saturated α-SiW12 clusters and [Cu2Cl2(tpy)2]2+ motifs. Compounds 13 exhibit bifunctional electro-catalytic behaviors for not merely reduction of nitrite but also oxidation of ascorbic acid. Electrocatalytic tests make clear that Sm-substituted hybrid based on POWs exhibits better activity than that for Eu-substitued/statured Keggin hybrids for electrocatalytic reduction of nitrite, statured Keggin hybrid shows better electro-catalytic performance for oxidations of ascorbic acid than those for Ln-substituted hybrids. The differences of electro-catalytic performances among three hybrids should be attributing to the distinctions of structures and electrochemical properties.

Graphical Abstract

Three inorganic-organic hybrids based on monovacant/saturated polyoxotungstates and 3d–4f metal chlorides were fabricated in the same POM/Ln/Cu-tpy reaction systems by adjusting pH. Compounds 1 and 2 display 1D circle-connecting-circle chain structure featured by {Ln–α–SiW11} polyxoanion clusters and {Cu/tpy} units, Compound 3 with 3D supramolecular structure consists of saturated α-SiW12 clusters and [Cu2Cl2(tpy)2]2+ motifs. Cyclic voltammetries of n-CPEs (n = 13) displayed bifunctional electrocatalytic activities toward reduction of nitrite and oxidation of ascorbic acid.

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中文翻译:

由Ln取代的单空位/饱和的Keggin多氧钨酸盐和Cu-Terpyridine Chlorides阻止的双功能电催化剂

摘要

基于monovacant /饱和polyoxotungstates和3d-4F金属氯化物三无机-有机杂化:[铜2(TPY)2 ] [钐(H 2 O)3 K(α-HSiW 11 ö 39)]氯·2H 2 O(1),[铜2(TPY)2 ] [Eu的(H 2 O)3 K(α-HSiW 11 ö 39)]氯·2H 2 O(2),铜44(TPY)4(α-硅钨酸12 O 40)]·2H 2 O(3)(tpy = 2,2':6',2''-terpyridine)在相同的POW / Ln / Cu-tpy反应体系中通过调节pH值制备。化合物12表现出以{Ln–α–SiW 11 }聚氧阴离子簇和{Cu / tpy}单元为特征的1D环-连接-环链结构。化合物3与三维超分子结构由饱和α-硅钨酸的12簇和物[Cu 22(TPY)2 ] 2+的基序。化合物1 - 3具有双功能的电催化行为,不仅可以还原亚硝酸盐,还可以氧化抗坏血酸。电催化测试清楚地表明,基于POWs的Sm取代的杂化物对Eu取代/固定的Keggin杂化物的亚硝酸盐电催化还原表现出更好的活性,固定的Keggin杂化物对抗坏血酸的氧化表现出比Ln-的更好的电催化性能。取代的杂种。三种杂化体之间电催化性能的差异应归因于结构和电化学性能的差异。

图形概要

在相同的POM / Ln / Cu-tpy反应体系中,通过调节pH值,制备了三种基于单空位/饱和多氧钨酸盐和3d-4f金属氯化物的无机-有机杂化物。化合物12显示1D圆连接圈链结构由{LN-α-硅钨酸功能11 } polyxoanion簇和{铜/ TPY}单位,化合物3与三维超分子结构由饱和的α-硅钨酸12簇和物[Cu 2个Cl 2(tpy)2 ] 2+个图案。的环状伏安法ñ -CPEs(Ñ = 1 - 3)显示出对亚硝酸盐还原和抗坏血酸氧化的双功能电催化活性。

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更新日期:2018-05-30
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