Atomic-level chelation engineered Ni-salicylate MOFs with hierarchical nanobelt assemblies for selective glucose electrooxidation

IF 7.7 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY
Min Wang  (, ), Yuan Li  (, ), Sicong Zhang  (, ), Xinyu Qin  (, ), Huan Pang  (, ), Qing Li  (, )
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Abstract

By employing a salicylate coordination strategy to precisely modulate the microenvironment of nickel active sites, a hierarchically porous nickel salicylate (Ni-SA) metal-organic framework (MOF) was constructed for efficient electrocatalytic glucose oxidation. The ortho-hydroxy-carboxylate chelation directs the atomic-level organization of Ni2+ sites within nanobelt assemblies, thereby maximizing active site accessibility. Robust Ni–O coordination further stabilized Ni3+ intermediates during C–H bond cleavage, leading to remarkable catalytic stability. As a result, the optimized Ni-SA-2 catalyst achieved outstanding sensing performance, with a high sensitivity of 5.97 mA mM−1 cm−2 and a low detection limit of 0.71 µM (signal-to-noise ratio (S/N) = 3), alongside 85.4% current retention after 8 h continuous operation. Significantly, this design paradigm demonstrates universal applicability as evidenced by successful extension to isostructural M-SA analogs (M = Co, Fe, Cr, Mn) under identical synthetic conditions, ultimately establishing metal-salicylate frameworks as a versatile electrocatalyst platform.

原子水平螯合工程镍水杨酸mof与分层纳米带组件选择性葡萄糖电氧化
采用水杨酸配位策略精确调节镍活性位点的微环境,构建了层次化多孔水杨酸镍(Ni-SA)金属有机骨架(MOF),用于高效电催化葡萄糖氧化。邻羟基羧酸螯合作用指导纳米带内Ni2+位点的原子级组织,从而最大化活性位点的可及性。强有力的Ni-O配位进一步稳定了C-H键裂解过程中的Ni3+中间体,从而获得了显著的催化稳定性。结果表明,优化后的Ni-SA-2催化剂具有出色的传感性能,灵敏度高达5.97 mA mM−1 cm−2,检测限低至0.71µM(信噪比(S/N) = 3),连续工作8 h后电流保持率为85.4%。值得注意的是,该设计范式具有普遍适用性,在相同的合成条件下成功地扩展到M- sa类似物(M = Co, Fe, Cr, Mn),最终建立了金属-水杨酸酯框架作为多功能电催化剂平台。
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来源期刊
Science China Materials
Science China Materials Materials Science-General Materials Science
CiteScore
11.40
自引率
7.40%
发文量
949
期刊介绍: Science China Materials (SCM) is a globally peer-reviewed journal that covers all facets of materials science. It is supervised by the Chinese Academy of Sciences and co-sponsored by the Chinese Academy of Sciences and the National Natural Science Foundation of China. The journal is jointly published monthly in both printed and electronic forms by Science China Press and Springer. The aim of SCM is to encourage communication of high-quality, innovative research results at the cutting-edge interface of materials science with chemistry, physics, biology, and engineering. It focuses on breakthroughs from around the world and aims to become a world-leading academic journal for materials science.
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