Sustainable and scalable natural fiber welded palladium-indium catalysts for nitrate reduction
Sustainable and scalable natural fiber welded palladium-indium catalysts for nitrate reduction
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DOI：
10.1016/j.apcatb.2017.09.029
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发表时间：
2018-02
影响因子：
22.1
通讯作者：
D. Durkin;Tao Ye;Jonglak Choi;K. Livi;H. Long;P. Trulove;D. Fairbrother;L. Haverhals;Danmeng Shuai
中科院分区：
文献类型：
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作者：
D. Durkin;Tao Ye;Jonglak Choi;K. Livi;H. Long;P. Trulove;D. Fairbrother;L. Haverhals;Danmeng Shuai
在这项工作中，我们展示了通过天然纤维焊接（NFW）将木质纤维素支撑的钯铟（Pd-In）纳米颗粒焊接到亚麻纱线上来生产活性，耐用，可持续的水处理催化剂。首先，Pd-In催化剂通过初始润湿到亚麻球磨粉末上来合成。我们的方法保留了木质纤维素，产生小的（5-10 nm），近球形的结晶纳米粒子的Pd-In合金和均匀的Pd-In金属组合物在整个纤维。硝酸盐还原测试确定了最佳Pd-In催化剂组合物（相对于木质纤维素为5重量% Pd和1.2重量% In）的存在以获得最大反应性;最具反应性的Pd-In催化剂的反应性是使用相同方法沉积在木质纤维素上的表现最佳的Pd-Cu纳米颗粒的10倍。这种改进的性能很可能是由于合金化的Pd-In纳米颗粒在整个载体中更均匀的分布。硝酸盐还原试验和X射线光电子能谱深度剖析老化的Pd-In催化剂表明，它们保持稳定，并在空气中在室温下长期储存期间没有失去反应活性。接下来，优化的Pd-In催化剂被纤维焊接到亚麻纱线上，使用定制的纱线涂层系统和控制催化剂负载的新型可扩展工艺，将Pd-In催化剂涂层传递到纱线表面上。这种纤维焊接的Pd-In催化剂纱线被集成到一种新型的水处理反应器中，并在超纯水中进行了四个月和超过180小时的硝酸盐还原试验。在该评估期间，纤维焊接的催化剂保持其反应性，金属浸出可忽略不计。当在未处理或（部分）处理的饮用水和废水中进行测试时，纤维焊接的催化剂是耐用和稳定的，并且它们的性能不受复杂沃茨中的成分（例如碱度、有机物）的显著影响。我们的研究展示了一种创新的，可扩展的方法，通过NFW设计和实施强大的，可持续的木质纤维素支持的催化剂，具有增强的反应性，能够在复杂的水化学中进行水净化。
In this work, we demonstrate the production of reactive, robust, sustainable catalysts for water treatment created throughNatural Fiber Welding(NFW) of lignocellulose-supported palladium-indium (Pd-In) nanoparticles onto linen yarns. First, Pd-In catalysts were synthesized by incipient wetness onto ball-milled powders of linen. Our process preserved the lignocellulose, yielding small (5–10 nm), near-spherical crystalline nanoparticles of Pd-In alloy and a uniform Pd-In metal composition throughout the fibers. Nitrate reduction tests identified the existence of an optimum Pd-In catalyst composition (5 wt% Pd and 1.2 wt% In with respect to lignocellulose) for maximum reactivity; the most reactive Pd-In catalyst was 10 times more reactive than the best performing Pd-Cu nanoparticles deposited on lignocellulose using the same approach. This improved performance was most likely due to more uniform distribution of alloyed Pd-In nanoparticles throughout the support. Nitrate reduction tests and X-ray photoelectron spectroscopy depth profiling of aged Pd-In catalysts showed that they remained stable and lost no reactivity during extended storage in air at room temperature. Next, the optimized Pd-In catalyst was fiber-welded onto linen yarns, using a custom-built yarn-coating system and a novel, scalable process that controlled catalyst loading, delivering a Pd-In catalyst coating onto the yarn surface. This fiber-welded Pd-In catalyst yarn was integrated into a novel water treatment reactor and evaluated during four months and more than 180 h of nitrate reduction tests in ultrapure water. During this evaluation, the fiber-welded catalysts maintained their reactivity with negligible metal leaching. When tested in raw or (partially) treated drinking water and wastewater, the fiber-welded catalysts were robust and stable, and their performance was not significantly impacted by constituents in the complex waters (e.g. alkalinity, organic matter). Our research demonstrates an innovative, scalable approach through NFW to design and implement robust, sustainable lignocellulose-supported catalysts with enhanced reactivity capable of water purification in complex water chemistries.