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題名 | The Electrocatalysis of Sulfite Oxidation and Reduction and Catalytic Autoxidation of Sulfite by Water-soluble Iron Porphyrin Fe(2-TMPyP)=水溶性鐵紫質Fe(2-TMPyP)對亞硫酸根的電催化氧化反應、還原反應及催化自動氧化反應 |
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作者 | 陳生明; |
期刊 | 臺北技術學院學報 |
出版日期 | 19960700 |
卷期 | 29:2 1996.07[民85.07] |
頁次 | 頁31-64 |
分類號 | 341.393 |
語文 | eng |
關鍵詞 | 水溶性鐵紫質; 亞硫酸根; 電催化氧化反應; 還原反應; 催化自動氧化反應; |
中文摘要 | 水溶性鐵紫質Fe(2-TMPyp)對SO32-的電催化氧化及還原反應有效。利用電化學 方法及光譜方法探討Fe(2-TMPyp)與SO32-,SH-,及其共軛酸鹼的氧化還原性質。FeIII( 2-TMPyP)在水溶液中能被NaSH還原成為FeII(2-TMPyP)(OH)及FeII(2-TMPyp)(H2O) ,也會與HSO3反應形成FeII(2-TMPyP)(SO32-)配位化合物。FeII(2-TMPyP)(SO32-) 在較鹼性溶液會與OH-反應生成FeII(2-TMPyp)(OH)。利用大體積電解,由離子色層分析 法得到Fe(2-TMPyP)電催化氧化SO32-的產物僅有SO12-。Fe(2-TMpyP)電催化還原SO32- 會生成HS-,H2S等產物。催化劑能完全再生。鐵紫質Fe(2-TMPyP)能與SO52-在除氧的情況 或在SO32-與氧共存的水溶液中反應生成穩定四價鐵紫質。SO32-在含氧溶液中能經由Fe(2 -TMPyP)的催化自動氧化反應快速生成SO42-。Fe(2-TMPyP)能電催化氧化H2S或HS-成為聚 合硫。 |
英文摘要 | The Electrocatalyic oxidation and reduction and catalytic autoxidation of SO32- by Fe(2-TMPyp) were investigated at room temperature in aqueous solution. The chemical reaction for the formation complex of FeII(2-TMPyP) with SO32- and the redox chemistry of Fe(2-TMPyP) with either SO32-, or HS-, or their conjugate acids or bases were determined by spectrophotometry and electrochemical method. FeIII(2-TMPyP) could be reduced by NaSH in a wide range of pH values. The results clearly demonstrate that FeII(2-TMPyP) reacted with SO32- at pH<11 forms FeII(2-TMPyp)(SO32-). At pH>11 FeII(2-TMPyP)(OH) is formed. The products formed in the electrocatalytic reaction by bulk electrolysis were determined by ion chromatography. Sulfate was the only product and no S2O62- was detected in the electrocatalytic oxidation of SO32- by Fe(2-TMPyP). The primary products of the electrocatalytic reduction of HSO3- by Fe(2-TMPyP) are S2O32- and Sx. H2S and SO42- are alsd Produced, in small amounts. FeIII(2-TMPyP) will be reduced to FeII(2-TMPyP) by both HSO3- and H2S, H2S is produced from the electrocatalytic reduction of HSO3-. The stable iron(IV) porphyrins, FeIV(O)(2- TMPyP) and (OH)FeIV(O)(2-TMPyP), can be produced by the chemical reaction of FeIII(2-TMPyP) with both HSO5 in the absence of oxygen and SO32- in presence of oxygen. FeII(2-TMPyP) can undergo electrocatalytic HS- oxidation to Sx2- in basic aqueous solution. Fe(2-TMPyP) acts as a catalyst in the autoxidation of SO32- to sulfate in the presence of oxygen. |
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