Water oxidation electrocatalysis by a zeolitic imidazolate framework.
Water oxidation electrocatalysis by a zeolitic imidazolate framework.
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DOI：
10.1039/c4nr02399d
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发表时间：
2014-08
期刊：
影响因子：
6.7
通讯作者：
Sibo Wang;Y. Hou;Sen Lin;Xinchen Wang
中科院分区：
文献类型：
--
作者：
Sibo Wang;Y. Hou;Sen Lin;Xinchen Wang
寻找高效的水氧化催化剂（WOCs）在能源和环境领域具有重要意义，但目前还没有在酸性和碱性条件下工作的良好非贵金属催化剂。近年来，钴基络合/固体催化剂得到了广泛的研究。本文介绍了一种新型的钴基WOC，该WOC由金属有机骨架制成，其中钴中心的氧化还原功能被咪唑酸盐连接剂修饰，以促进质子转移过程。这种含钴的沸石咪唑盐框架（Co-ZIF-9）首次被证明可以在很宽的pH范围内电催化出氧反应。通过理论计算发现，该催化剂能够通过将oh基团结合到具有低激活障碍的金属位上来激活水分子，而消除的质子则被附近的苯并咪唑基序所接受。这使得Co-ZIF-9能够有效地进行电化学析氧反应。
The search for efficient water oxidation catalysts (WOCs) is of paramount importance in energy and environmental fields, but there exists no good non-noble catalyst that works under acidic and alkaline conditions. Intensive investigations have recently focused on cobalt based complex/solid catalysts. Here, we have introduced a new type of cobalt-based WOC made of metal-organic frameworks where the redox function of cobalt centres was modified by imidazolate linkers for facilitating the proton transfer process. This cobalt-containing zeolitic imidazolate framework (Co-ZIF-9) has been demonstrated for the first time to electrocatalyze the oxygen evolution reaction in a wide pH range. The catalyst was found by theoretical calculation to be capable of activating the water molecule via binding the OH-group to the metal sites with low activation barriers, while the eliminated proton was accepted by the nearby benzimidazolate motifs. This allows Co-ZIF-9 to work effectively for the electrochemical oxygen-evolution reaction.