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ZnMn2O4 nanorods: an effective Fenton-like heterogeneous catalyst with t2g3eg1 electronic configuration†
Catalysis Science & Technology ( IF 4.4 ) Pub Date : 2018-04-23 00:00:00 , DOI: 10.1039/c8cy00436f Maoqin Qiu 1, 2, 3, 4 , Zhangxian Chen 1, 2, 3, 4 , Zeheng Yang 1, 2, 3, 4 , Wenming Li 1, 2, 3, 4 , Yuan Tian 1, 2, 3, 4 , Weixin Zhang 1, 2, 3, 4 , Yishu Xu 1, 2, 3, 4 , Hansong Cheng 5, 6, 7, 8, 9
Catalysis Science & Technology ( IF 4.4 ) Pub Date : 2018-04-23 00:00:00 , DOI: 10.1039/c8cy00436f Maoqin Qiu 1, 2, 3, 4 , Zhangxian Chen 1, 2, 3, 4 , Zeheng Yang 1, 2, 3, 4 , Wenming Li 1, 2, 3, 4 , Yuan Tian 1, 2, 3, 4 , Weixin Zhang 1, 2, 3, 4 , Yishu Xu 1, 2, 3, 4 , Hansong Cheng 5, 6, 7, 8, 9
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Fenton-like catalysis is promising in the treatment of organic-containing wastewater owing to easy separation of solid catalysts, wide working pH range, and high efficiency. Although α-Mn2O3 with Mn3+ in t2g3eg1 electronic configuration displays high activity in photocatalytic oxidation of water, it is not preferred as a Fenton-like catalyst due to its low phase-transition temperature. Herein, we developed a Fenton-like catalyst with both high activity and stability. Two catalysts, namely, spinel ZnMn2O4 and ZnMnO3 nanorods were synthesized by a facile co-precipitation method. Experimental results indicate that the two Mn-containing catalysts have similar rod-like morphology, but with different crystallographic structures and oxidation states of Mn. DFT calculations suggest t2g3eg1 electron configuration of Mn in ZnMn2O4 with strong Jahn–Teller distortion of MnO6 units. ZnMn2O4 nanorod Fenton-like catalyst displays high activity in the degradation of methyl violet with a degradation ratio of 100% at 120 min and a TOC removal rate near 90% after 240 min. ˙OH and ˙OOH/˙O2− reactive radicals generated in the catalytic system were studied by EPR spectroscopy. The ZnMn2O4 nanorods exhibited much better catalytic performance than ZnMnO3 nanorods. The t2g3eg1 configuration of Mn in spinel ZnMn2O4, facilitating the dissociation of various oxygen-containing radicals through strong JT distortion, is responsible for its higher catalytic activity.
中文翻译：
ZnMn 2 O 4纳米棒：一种有效的Fenton型非均相催化剂，其电子构型为t 2g 3 e g 1 †
由于易于分离固体催化剂，宽的工作pH范围和高效率，类Fenton催化法在处理有机废水中很有前途。虽然α-Mn系2 ö 3与锰3+在吨2克3 é克1个电子结构显示高的水光催化氧化，它不是优选的，因为一个类芬顿催化剂由于其低的相转变温度。本文中，我们开发了既具有高活性又具有稳定性的类芬顿催化剂。两种催化剂，即尖晶石ZnMn 2 O 4和ZnMnO 3纳米棒通过简便的共沉淀法合成。实验结果表明，两种含锰催化剂具有相似的棒状形态，但具有不同的晶体结构和锰的氧化态。DFT计算表明ZnMn 2 O 4中Mn的t 2g 3 e g 1电子构型具有MnO 6单位的强Jahn-Teller畸变。ZnMn 2 O 4纳米棒芬顿样催化剂在甲基紫的降解中表现出高活性，在120分钟时的降解率为100％，在240分钟后的TOC去除率接近90％。OH和OOH / O 2 -通过EPR光谱研究了催化体系中产生的反应性自由基。ZnMn 2 O 4纳米棒表现出比ZnMnO 3纳米棒更好的催化性能。尖晶石ZnMn 2 O 4中Mn的t 2g 3 e g 1构型通过强JT变形促进各种含氧自由基的离解，是其较高的催化活性的原因。
更新日期：2018-04-23
中文翻译：
ZnMn 2 O 4纳米棒：一种有效的Fenton型非均相催化剂，其电子构型为t 2g 3 e g 1 †
由于易于分离固体催化剂，宽的工作pH范围和高效率，类Fenton催化法在处理有机废水中很有前途。虽然α-Mn系2 ö 3与锰3+在吨2克3 é克1个电子结构显示高的水光催化氧化，它不是优选的，因为一个类芬顿催化剂由于其低的相转变温度。本文中，我们开发了既具有高活性又具有稳定性的类芬顿催化剂。两种催化剂，即尖晶石ZnMn 2 O 4和ZnMnO 3纳米棒通过简便的共沉淀法合成。实验结果表明，两种含锰催化剂具有相似的棒状形态，但具有不同的晶体结构和锰的氧化态。DFT计算表明ZnMn 2 O 4中Mn的t 2g 3 e g 1电子构型具有MnO 6单位的强Jahn-Teller畸变。ZnMn 2 O 4纳米棒芬顿样催化剂在甲基紫的降解中表现出高活性，在120分钟时的降解率为100％，在240分钟后的TOC去除率接近90％。OH和OOH / O 2 -通过EPR光谱研究了催化体系中产生的反应性自由基。ZnMn 2 O 4纳米棒表现出比ZnMnO 3纳米棒更好的催化性能。尖晶石ZnMn 2 O 4中Mn的t 2g 3 e g 1构型通过强JT变形促进各种含氧自由基的离解，是其较高的催化活性的原因。
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