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The Marriage of Hydrazone-Linked Covalent Organic Frameworks and MXene Enables Efficient Electrocatalytic Hydrogen Evolution
Small Structures ( IF 13.9 ) Pub Date : 2023-09-26 , DOI: 10.1002/sstr.202300279 Chenyu Ma 1 , Haiyan He 1 , Jinlong Qin 1 , Lang Luo 1 , Yue Lan 1 , Jian Zhang 2 , Lu Yang 1 , Quanguo Jiang 1 , Huajie Huang 1
Small Structures ( IF 13.9 ) Pub Date : 2023-09-26 , DOI: 10.1002/sstr.202300279 Chenyu Ma 1 , Haiyan He 1 , Jinlong Qin 1 , Lang Luo 1 , Yue Lan 1 , Jian Zhang 2 , Lu Yang 1 , Quanguo Jiang 1 , Huajie Huang 1
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Electrochemical water splitting is long regarded as a green and feasible pathway to realize the scalable hydrogen production, while the overall hydrogen evolution reaction (HER) efficiency is largely dependent on the electrocatalytic ability of the cathode catalysts. Herein, the in situ growth of hydrazone-linked covalent organic framework (COF-42) nanocrystals with a unique nanoflower-shaped morphology on 2D ultrathin Ti3C2Tx MXene nanosheets (COF/Ti3C2Tx) is achieved through a convenient and robust stereoassembly strategy. Strikingly, the marriage of COF-42 and Ti3C2Tx nanosheets not only offers multiscale porous channels for the fast transportation of electrolyte and electrons, but also enables the full exposure and activation of numerous catalytically active centers. As a consequence, the optimized COF/Ti3C2Tx nanoarchitecture displays exceptional HER properties in terms of a very low onset potential of 19 mV, a small Tafel slope of 50 mV dec−1 as well as reliable long-term durability, which are comparable to those of commercial Pt/C catalyst. Density functional theory calculations further disclose that the rational combination of COF-42 with Ti3C2Tx provides more diversified active positions with appropriate ΔGH values, thus leading to a boosted hydrogen generation rate.
中文翻译：
腙连接的共价有机框架和 MXene 的结合可实现高效的电催化析氢
电化学水分解长期以来被认为是实现规模化制氢的绿色可行途径，而整体析氢反应（HER）效率在很大程度上取决于阴极催化剂的电催化能力。在此，在二维超薄 Ti 3 C 2 T x MXene 纳米片（COF/Ti 3 C 2 T x ）上原位生长具有独特纳米花形形貌的腙连接的共价有机骨架（COF- 42 ）纳米晶体是通过方便且强大的立体组装策略。引人注目的是，COF-42 和 Ti 3 C 2 T x纳米片的结合不仅为电解质和电子的快速传输提供了多尺度多孔通道，而且还使得众多催化活性中心能够充分暴露和激活。因此，优化的 COF/Ti 3 C 2 T x纳米结构表现出优异的 HER 性能，包括 19 mV 的极低起始电位、50 mV dec -1的小塔菲尔斜率以及可靠的长期耐用性，与商业 Pt/C 催化剂相当。密度泛函理论计算进一步表明，COF-42与Ti 3 C 2 T x的合理组合提供了更多样化的活性位置和合适的Δ G H值，从而提高了产氢速率。
更新日期：2023-09-26
中文翻译：
腙连接的共价有机框架和 MXene 的结合可实现高效的电催化析氢
电化学水分解长期以来被认为是实现规模化制氢的绿色可行途径，而整体析氢反应（HER）效率在很大程度上取决于阴极催化剂的电催化能力。在此，在二维超薄 Ti 3 C 2 T x MXene 纳米片（COF/Ti 3 C 2 T x ）上原位生长具有独特纳米花形形貌的腙连接的共价有机骨架（COF- 42 ）纳米晶体是通过方便且强大的立体组装策略。引人注目的是，COF-42 和 Ti 3 C 2 T x纳米片的结合不仅为电解质和电子的快速传输提供了多尺度多孔通道，而且还使得众多催化活性中心能够充分暴露和激活。因此，优化的 COF/Ti 3 C 2 T x纳米结构表现出优异的 HER 性能，包括 19 mV 的极低起始电位、50 mV dec -1的小塔菲尔斜率以及可靠的长期耐用性，与商业 Pt/C 催化剂相当。密度泛函理论计算进一步表明，COF-42与Ti 3 C 2 T x的合理组合提供了更多样化的活性位置和合适的Δ G H值，从而提高了产氢速率。
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