高熵金属有机框架衍生物加速不对称酸/碱 N2 电固定,Carbon Energy

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高熵金属有机框架衍生物加速不对称酸/碱 N2 电固定
Carbon Energy ( IF 19.5 ) Pub Date : 2022-10-17 , DOI: 10.1002/cey2.263
Yuntong Sun ₁ , Wenqiang Wu ₁ , Lei Yu ₁ , Shuaishuai Xu ₁ , Yuxiang Zhang ₁ , Licheng Yu ₁ , Baokai Xia ₁ , Shan Ding ₁ , Ming Li ₁ , LiLi Jiang ₁ , Jingjing Duan ₁ , Junwu Zhu ₁ , Sheng Chen ₁

Affiliation

高熵材料由五种或更多种等摩尔或接近等摩尔浓度的金属元素在一个晶体结构中组成，为许多应用提供了卓越的结构特性。尽管之前报道过熵驱动的稳定机制，但许多高熵材料在操作条件下仍倾向于分解产生各种衍生物。在这项研究中，我们使用基于过渡金属（Ni、Co、Ni、Zn、V）的高熵金属有机框架（HE-MOFs）作为前体，在酸/碱处理下生产不同的衍生物。我们已经表明，HE-MOF 和衍生物已显示出对 N _{2有利的动力学}在不同 pH 电解质中的电固定，特别是酸性介质中的阴极氮还原反应和碱性介质中的阳极析氧反应。为了缓冲 pH 失配，我们进一步使用双极膜构建了一个不对称酸/碱装置原型。正如预期的那样，该原型显示出显着的活性，NH ₃产率为42.76 μg h ⁻¹ mg ⁻¹，法拉第效率为14.75%，能量效率为2.59%，分别是其对称的14.4和4.4倍。分别对应酸性和碱性。

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Asymmetric acidic/alkaline N2 electrofixation accelerated by high-entropy metal–organic framework derivatives

High-entropy materials are composed of five or more metal elements with equimolar or near-equimolar concentrations within one crystal structure, which offer remarkable structural properties for many applications. Despite previously reported entropy-driven stabilization mechanisms, many high-entropy materials still tend to decompose to produce a variety of derivatives under operating conditions. In this study, we use transition-metal (Ni, Co, Ni, Zn, V)-based high-entropy metal–organic frameworks (HE-MOFs) as the precursors to produce different derivatives under acidic/alkaline treatment. We have shown that HE-MOFs and derivatives have shown favorable kinetics for N₂ electrofixation in different pH electrolytes, specifically cathodic nitrogen reduction reaction in acidic media and anodic oxygen evolution reaction in alkaline media. To buffer the pH mismatch, we have further constructed an asymmetric acidic/alkaline device prototype by using bipolar membranes. As expected, the prototype showed remarkable activities, with an NH₃ yield rate of 42.76 μg h⁻¹ mg⁻¹, and Faradaic efficiency of 14.75% and energy efficiency of 2.59%, which are 14.4 and 4.4 times larger than those of its symmetric acidic and alkaline counterparts, respectively.

更新日期：2022-10-17

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