Molybdenum-Catalyzed Perchlorate Reduction: Robustness, Challenges, and Solutions
Molybdenum-Catalyzed Perchlorate Reduction: Robustness, Challenges, and Solutions
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DOI：
10.1021/acsestengg.1c00290
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发表时间：
2022-02-11
影响因子：
7.1
通讯作者：
Liu, Jinyong
中科院分区：
文献类型：
--
作者：
Ren, Changxu;Bi, Eric Y.;Liu, Jinyong
我们最近研制了一种高活性的配体活化(L)Mo-Pd/C催化剂(L=4，4‘-二氨基-2，2’-联吡啶)，用于高氯酸水溶液(ClO_4-)的室温还原。本文报道了该催化剂与离子交换树脂再生废盐水中ClO4处理密切相关的一系列令人满意的性能。在浓盐和腐植酸存在下，催化剂对ClO4-有一定的抑制作用，但在几个小时内完成ClO4-还原，负载量在0.2~2g/L之间可调。催化剂没有因多个100 mM ClO4-的高氧化压力而失活。用In-Pd/Al_2O_3对卤水进行前处理，解决了硝酸盐失活的难题。通过在pH值为12的条件下对Pd/C进行再生，克服了配体加氢造成的活性损失。我们还对催化剂配方进行了优化，在不牺牲活性的情况下节省了70%的Pd。(L)Mo-Pd/C的催化性能显著提高，对环境的不利影响降低，使其在ClO4还原方面与微生物反应器竞争。我们展示了配位化学在环境技术创新中的力量，并期待这种催化剂能够促进ClO4选择性树脂的再利用，用于可持续的水处理。
We have recently developed a highly active ligandenabled (L)Mo-Pd/C catalyst (L = 4,4 '-diamino-2,2 '-bipyridine) for aqueous perchlorate (ClO4-) reduction with 1 atm H-2 at room temperature. This study reports on a series of satisfactory properties of this catalyst closely relevant to ClO4- treatment in waste brines resulting from ion-exchange resin regeneration. In the presence of concentrated salts and humic acid, the catalyst experienced limited inhibition but completed ClO4- reduction in a few hours with an adjustable loading between 0.2 and 2 g/L. The catalyst was not deactivated by the high oxidative stress from multiple spikes of 100 mM ClO4-. The challenge of deactivation by nitrate was solved by pretreating the brine with In-Pd/Al2O3. The loss of activity upon ligand hydrogenation was overcome by regenerating the Pd/C at pH 12. We also optimized the catalyst formulation and saved 70% of Pd without sacrificing the activity. The substantially enhanced performance and lowered adverse environmental impacts of (L)Mo-Pd/C make the catalytic treatment competitive to microbial reactors for ClO4- reduction. We showcase the power of coordination chemistry in environmental technology innovation and expect this catalyst to promote the reuse of ClO4--selective resins for sustainable water treatment.