| Co(C3H6NS2)3·C6H12N2S3单晶的制备及催化性能的研究 |
| 摘要点击 3113 全文点击 2068 投稿时间：2008-01-21 修订日期：2008-03-10 |
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| 中文关键词 单晶 非均相Fenton法 高级氧化法 染料废水 降解 |
| 英文关键词 single crystal heterogeneous Fenton advanced oxidation processes dye wastewater degradation |
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| 中文摘要 |
| 采用常温饱和溶液蒸发法，一硫化四甲基秋兰姆与钴(Ⅱ)发生原位反应得到一种新型非均相Fenton催化剂单晶Co(C3H6NS2)3·C6H12N2S3；通过单晶X衍射、红外光谱和C、N和H元素分析对该单晶结构进行了表征；该单晶的空间群为P-1，在不对称单元中有1个Co(Ⅲ)中心，3个新配体C3H7NS2和1个TMTM；Co(Ⅲ)呈现出稍微偏斜的八面体的配位几何构型.利用该单晶催化氧化降解了直接蓝6和直接绿28；结果显示，在酸性和碱性条件下，染料的降解率和矿化率都较高，这是因为活性中心Co(Ⅲ)提高了H2O2的效率.当投加量在1 200～1 600 mg·L-1之间时，处理90 min后，直接蓝6和直接绿28的降解效率可分别达到94.39%和94.78%.相比之下，不加该单晶光催化剂，其它条件完全相同时，处理90 min后2种染料的降解率均不到45%，降解缓慢.使用后的单晶，通过过滤，可反复使用，有利于降低处理成本.此外还研究了催化反应的动力学，反应遵从Langmuir-Hinshelwood动力学模型；2种染料降解反应速率常数k分别为3.03×102和6.25×102 mg·(L·min)-1，吸附常数K分别为1.52×10-4和7.23×10-5 L·mg-1. |
| 英文摘要 |
| A novel heterogeneous Fenton catalyst Co(C3H6NS2)3·C6H12N2S3 was synthesized in an in-situ reaction with tetramethyl thiuram monosulfide and cobalt(Ⅱ) slowly evaporating at room temperature. Its structure was characterized by single crystal X-ray diffraction(XRD). Infrared spectrum (IR) and CNH elemental analysis. The catalyst crystallizes in P-1 space group with one cobalt(Ⅲ) ion, three new ligands and one dissociated TMTM molecule in the asymmetric unit, presenting a distorted octahedral geometry. Using the single crystal, the results of photocatalytic degradation of direct orchid 6 and direct green 28, as a model reaction, show that when adding between 1 600 and 1 200 mg·L-1 of photocatalys, the degradation rate of direct orchid 6 and direct green 28 reach 94.39% and 94.78%. The single crystal by filtered after the Fenton reaction can be used repeatedly. Thus the cost of water treatment was reduced. The photocatalytic degradation of direct orchid 6 and direct green 28 have been experimentally demonstrated to follow the Langmuir-Hinshelwood kinetic model, meanwhile the reaction rate constants［3.03×102 and 6.25×102 mg·(L·min)-1］ and the adsorption constants(1.52×10-4 and 7.23×10-5 L·mg-1)have been determined, respectively. |
