Key Takeaways & Executive Findings
- •• • Ni-SA-2 exhibits a sensitivity of 5.97 mA mM−1 cm−2 and a detection limit of 0.71 μM (S/N = 3), enabling trace-level glucose quantification in clinical diagnostics and food quality control. • • The catalyst retains 85.4% of its initial current after 8 h continuous operation, indicating robust operational stability critical for long-term implantable or industrial sensors. • • The synthesis is extended to isostructural M-SA analogs (M = Co, Fe, Cr, Mn) under identical conditions, demonstrating a universal platform for tunable electrocatalyst design. • • The hierarchical nanobelt architecture maximizes active site accessibility and facilitates mass transport, directly improving reaction kinetics and sensor response time.
Abstract
A hierarchically porous nickel salicylate (Ni-SA) metal-organic framework (MOF) was constructed via a salicylate coordination strategy to precisely modulate the microenvironment of nickel active sites for efficient electrocatalytic glucose oxidation. The ortho-hydroxy-carboxylate chelation directs atomic-level organization of Ni2+ sites within nanobelt assemblies, maximizing active site accessibility. Robust Ni–O coordination stabilizes Ni3+ intermediates during C–H bond cleavage, leading to remarkable catalytic stability. The optimized Ni-SA-2 catalyst achieved a high sensitivity of 5.97 mA mM−1 cm−2 and a low detection limit of 0.71 μM (S/N = 3), with 85.4% current retention after 8 h continuous operation. 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, establishing metal-salicylate frameworks as a versatile electrocatalyst platform.
1. Introduction
Non-enzymatic electrochemical glucose sensors face a critical bottleneck: conventional nickel-based electrodes suffer from poor active-site utilization and insufficient stability under continuous operation, limiting sensitivity and longevity. The challenge is to engineer catalysts with precisely controlled coordination environments that enhance both intrinsic activity and structural robustness.
This work addresses this by employing a salicylate chelation strategy to construct Ni-MOFs with hierarchical nanobelt assemblies. The ortho-hydroxy-carboxylate coordination directs atomic-level organization of Ni2+ sites, while robust Ni–O bonds stabilize Ni3+ intermediates during glucose oxidation. This design not only maximizes active-site accessibility but also ensures high catalytic stability, offering a promising route to high-performance, durable glucose sensors.
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Min Wang, Yuan Li, Sicong Zhang, Xinyu Qin, Huan Pang, Qing Li (2026). Atomic-Level Chelation Engineered Ni-Salicylate MOFs with Hierarchical Nanobelt Assemblies for Selective Glucose Electrooxidation. SCIENCE CHINA Materials. https://doi.org/10.1007/s40843-025-3987-x
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Frequently Asked Questions
What is the underlying mechanism for the enhanced catalytic activity and stability of Ni-SA-2 compared to conventional nickel-based catalysts?
The ortho-hydroxy-carboxylate chelation in salicylate ligands directs the atomic-level organization of Ni2+ sites, maximizing active site accessibility. The robust Ni–O coordination stabilizes Ni3+ intermediates during C–H bond cleavage, which is the rate-determining step in glucose oxidation. This stabilization reduces overpotential and enhances catalytic turnover, while the hierarchical nanobelt structure provides short diffusion pathways and structural integrity, contributing to the observed 85.4% current retention after 8 h.
How does the sensitivity and detection limit of Ni-SA-2 compare to state-of-the-art non-enzymatic glucose sensors, and what are the implications for clinical diagnostics?
Ni-SA-2 achieves a sensitivity of 5.97 mA mM−1 cm−2 and a detection limit of 0.71 μM (S/N = 3). These metrics are competitive with or superior to many reported non-enzymatic sensors, which typically exhibit sensitivities in the range of 0.1–2 mA mM−1 cm−2 and detection limits above 1 μM. The low detection limit enables accurate glucose quantification in physiological ranges, crucial for diabetes management and point-of-care testing.
What is the practical scalability of the synthesis method for industrial production?
The synthesis is conducted under identical conditions for isostructural M-SA analogs (M = Co, Fe, Cr, Mn), indicating a simple, reproducible, and scalable protocol. The use of salicylate as a low-cost ligand and mild reaction conditions (likely solvothermal) suggests potential for scale-up. However, detailed yield and cost analysis are not provided in the abstract, so further economic assessment is required.
What are the potential failure mechanisms of Ni-SA-2 under prolonged operation, and how does the catalyst mitigate them?
Potential failure mechanisms include active-site leaching, structural collapse, and surface poisoning by reaction intermediates. The robust Ni–O coordination and hierarchical nanobelt assembly enhance structural stability, as evidenced by 85.4% current retention after 8 h. The porous structure may also facilitate desorption of products, reducing fouling. However, long-term stability beyond 8 h and resistance to chloride ions (common in biological fluids) are not reported and warrant further investigation.
How does the selectivity of Ni-SA-2 for glucose oxidation against interfering species (e.g., ascorbic acid, uric acid) compare to enzymatic sensors?
The abstract does not provide specific selectivity data. However, non-enzymatic sensors often rely on operating potential to minimize interference. The hierarchical nanobelt structure and tailored active sites may enhance intrinsic selectivity, but quantitative data on interference ratios are necessary. Typically, enzymatic sensors offer high selectivity but suffer from instability; Ni-SA-2's stability advantage could be offset by lower selectivity unless optimized.
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