Cheng Si Yuan,Yang Xi Nan,Tao Zhu,Wei Lian Tong,Zhao Wei Wei,Jiang Dao Fa,Jin Yan Mei,Gao Jie,Ma Pei Hua
Abstract The host–guest binding characteristics of cyclopentanocucurbit[6]uril (CyP 6 Q[6]) and cyanine dye trans -4-[4-(dimethylamino)styryl]-1-methylpyridinium iodide ( t -DSMI) have been studied. The results show that CyP 6 Q[6] and t -DSMI form a 1:1 inclusion system, generating strong fluorescence. On this basis, the fluorescent probe t -DSMI@CyP 6 Q[6] has been constructed, and its anion recognition ability has been investigated. In a neutral environment, BF 4 − , H 2 PO 4 − , and I − elicit obvious specific responses from the probe, since they have stronger binding forces. This probe shows greater sensitivity than the previously reported probe t -DSMI@HMeQ[6]. Graphic abstract Since the complex formed by CyP 6 Q[6] and t -DSMI can produce strong fluorescence at pH > 4.6, t -DSMI@CyP 6 Q[6] was constructed to recognize the anions at pH ≅ 5. The results show that in a near neutral environment, BF 4 − , H 2 PO 4 − , and I − elicit obvious specific responses from the probe.
Bo Zhang,Shiyu Ma,Xin Mi,Wenjia Xiao,Xinai Xiao,Jinjue Wang,Hui Zeng,Yuan Chang,Jungang Hou
The sluggish kinetics of both proton dissociation and proton migration during OER is identified as the key bottleneck. • High-pKa H 2 PO 4 − groups are incorporated into NiFe LDH to upshift the d-band center and optimize electronic structure. • H 2 PO 4 − groups function as proton ferry to facilitate O H bond cleavage and reduce the energy barrier. • A proton highway is constructed via the Grotthuss mechanism by mediating a hydrogen-bond-rich microenvironment. • Synergistic promotion of proton dissociation and migration leads to outstanding OER activity and stability. Alkaline water electrolysis represents a promising strategy for sustainable hydrogen production. However, its energy efficiency is significantly constrained by the inherently sluggish kinetics of proton dissociation and proton migration during oxygen evolution reaction (OER). To address this limitation, the H 2 PO 4 − groups with high pKa value were reasonably incorporated into the lattice of NiFe-layered double hydroxide (P-NiFe LDH), thus optimizing the electronic structure by upshifting the d -band centre to improve the mass transfer. Additionally, the H 2 PO 4 − groups also functioned as proton ferry groups, which facilitated the cleavage of O H bonds in key intermediates to reduce the energy barrier. The in-situ Raman spectra and DFT calculations further confirmed that the H 2 PO 4 − groups mediated the microenvironment rich in hydrogen bond network, thus constructing a highway for proton transport via the Grotthuss mechanism. Ultimately, the P-NiFe LDH demonstrated exceptional activity toward water oxidation, requiring only an overpotential of 283 mV at the current density of 100 mA cm −2 , while maintaining remarkable stability for over 50 h at 10 mA cm −2 . This work not only highlights the importance of synergistically promoting the process of proton dissociation and proton migration in OER, but also provides valuable insights for the design of high-performance OER electrocatalysts.
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