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使用催化和未催化的纳米级铁颗粒对无缓冲硝酸盐溶液进行化学还原。

Chemical reduction of an unbuffered nitrate solution using catalyzed and uncatalyzed nanoscale iron particles.

作者信息

Liou Ya Hsuan, Lo Shang-Lien, Lin Chin-Jung, Kuan Wen Hui, Weng Shih Chi

机构信息

Research Center for Environmental Pollution Prevention and Control Technology, Graduate Institute of Environmental Engineering, National Taiwan University, Taipei.

出版信息

J Hazard Mater. 2005 Dec 9;127(1-3):102-10. doi: 10.1016/j.jhazmat.2005.06.029. Epub 2005 Aug 2.

Abstract

Uncatalyzed and catalyzed nanoscale Fe(0) systems were employed for the denitrification of unbuffered 40 mgN L(-1) nitrate solutions at initial neutral pH. Compared to microscale Fe(0) (<100 mesh), the efficiency and rate of nitrate removal using uncatalyzed and catalyzed nano-Fe(0) were highly promoted, in which the maximum promoted rate was obtained using copper-catalyzed nano-Fe(0) (nano-Cu/Fe). Nitrate first-order degradation rate constants (k(obs)) decreased significantly (>70%) with aged nano-Fe(0) and aged nano-Cu/Fe, and were recovered with NaBH(4) as reductants at levels of about 85 and 75%, respectively. Activation energies (E(a)) of nitrate reduction over the temperature range of 10-60 degrees C were 42.5 kJ mol(-1) for microscale Fe(0), 25.8 kJ mol(-1) for nano-Fe(0) and 16.8 kJ mol(-1) for nano-Cu/Fe. Unlike microscale Fe(0), the kinetics of denitrification by nano-Fe(0) and nano-Cu/Fe began to show characteristics of mass transport in addition to chemical reaction control. Ammonium was the predominant end product in all the systems. However, as for nitrite, 40% of the degraded nitrate persisted in the nano-Cu/Fe system. Thus, relative to nano-Cu/Fe, nano-Fe(0) is a potential reductant for denitrification of groundwater as far as toxic nitrite generation is concern.

摘要

在初始中性pH值条件下,使用未催化和催化的纳米级零价铁体系对未缓冲的40 mgN L⁻¹硝酸盐溶液进行反硝化处理。与微米级零价铁(<100目)相比,未催化和催化的纳米零价铁去除硝酸盐的效率和速率得到了显著提高,其中使用铜催化的纳米零价铁(nano-Cu/Fe)时促进率最高。随着纳米零价铁和纳米铜/铁的老化,硝酸盐一级降解速率常数(k(obs))显著降低(>70%),分别以硼氢化钠作为还原剂时,其降解速率常数分别恢复到约85%和75%的水平。在10 - 60℃温度范围内,微米级零价铁还原硝酸盐的活化能(E(a))为42.5 kJ mol⁻¹,纳米零价铁为25.8 kJ mol⁻¹,纳米铜/铁为16.8 kJ mol⁻¹。与微米级零价铁不同,纳米零价铁和纳米铜/铁的反硝化动力学除了化学反应控制外,还开始表现出传质特征。铵是所有体系中的主要终产物。然而,对于亚硝酸盐,在纳米铜/铁体系中,40%降解的硝酸盐以亚硝酸盐形式存在。因此,就有毒亚硝酸盐的生成而言,相对于纳米铜/铁,纳米零价铁是地下水中反硝化的潜在还原剂。

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