Coordination Number Regulation of Molybdenum Single-Atom Nanozyme Peroxidase-like Specificity

Wang, Ying; Jia, Guangri; Cui, Xiaoqiang; Zhao, Xiao; Zhang, Qinghua; Gu, Lin; Zheng, Lirong; Li, Lu Hua; Wu, Qiong; Singh, David J.; Matsumura, Daiju; Tsuji, Takuya; Cui, Yi‐Tao; Zhao, Jingxiang; Zheng, Weitao

doi:10.1016/j.chempr.2020.10.023

Cited by 284 publications

(223 citation statements)

References 60 publications

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“…According to the reported nanozymes as POD mimics, it is commonly believed that POD‐like nanozymes can transform H 2 O 2 into active hydroxyl radicals (•OH), and abundant •OH can further oxidize allochroic agents. [ 43–46 ] Therefore, electron paramagnetic resonance (EPR) spectrum was used to probe •OH intermediates in the DCN‐catalyzed processes. As shown in Figure a, the characteristic peaks of •OH are detected in all groups.…”

Section: Resultsmentioning

confidence: 99%

Defect‐Engineered Nanozyme‐Linked Receptors

Wen

et al. 2021

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Though nanozymes are successfully applied in various areas, the increasing demands facilitate the exploitation of nanozymes possessing higher activity and more functions. Natural enzyme‐linked receptors (ELRs) are critical components for signal transductions in vivo by expressing activity variations after binding with ligands. Inspired by this, the defect‐engineered carbon nitrides (DCN) are reported to serve as nanozyme‐linked receptors (NLRs). For one thing, cyano defects increase the enzyme‐like activity by a factor of 109.5. For another, DCN‐based NLRs are constructed by employing cyano groups as receptors, and variable outputs are ensued upon the addition of ion ligands. Significantly, both the cascade effect and electronic effect are demonstrated to contribute to this phenomenon. Finally, NLRs are used for pattern recognition of metal ions, indicating the signal transduction ability of NLRs as well. This work not only provides great promise of defect engineering in nanozymes, but also contributes to the design of artificial ELRs.

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Section: Resultsmentioning

confidence: 99%

Defect‐Engineered Nanozyme‐Linked Receptors

Wen

et al. 2021

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“…S3 and Table S3). The coordination structure has a significant influence on catalytic performance [36][37], which is discussed in a later section.…”

Section: Resultsmentioning

confidence: 99%

Ionic-liquid-assisted synthesis of metal single-atom catalysts for benzene oxidation to phenol

Shen

Chen

et al. 2021

Sci. China Mater.

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Ionic liquids (ILs) have the advantages of low cost, eco-friendliness, abundant heteroatoms, excellent solubility, and coordinated ability with metal ions. These features make ILs a suitable precursor for fabricating metal singleatom catalysts (SACs). Herein, we prepared various metal single atoms anchored on ultrathin N-doped nanosheets (denoted as Cu 1 /NC, Fe 1 /NC, Co 1 /NC, Ni 1 /NC, and Pd 1 /NC) by direct pyrolysis using ILs and g-C 3 N 4 nanosheets as templates. Taking benzene oxidation to phenol with H 2 O 2 as a model reaction to evaluate their catalytic performance and potential applications, Cu 1 /NC calcined at 1000°C (denoted as Cu 1 /NC-1000) exhibits the highest activity with a turnover frequency of about 200 h −1 in the first 1 h at 60°C , which is better than that of most metal SACs reported in the literature. High benzene conversion of 82% with high phenol selectivity of 96% and excellent recyclability were achieved using the Cu 1 /NC-1000 catalyst. This study provides an efficient general strategy for fabricating SACs using ILs for catalytic applications.

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“…77 Other researchers also reached a similar conclusion that the lower coordination number in SACs indeed strengthened the adsorption of CO 2 RR intermediates. [78][79][80][81][82][83] 3.2.3. Effect of the coordinated nitrogen type on CO 2 reduction to CO. Four types of nitrogen atoms exist in SACs, namely pyridinic, pyrrolic, graphitic and oxidized N. The metal centers in SACs could be bonded with pyridinic N or pyrrolic N. The d-band center for pyrrolic-N coordinated metal sites is lower than that for pyridinic-N coordinated metal sites and thus pyrrolic-N coordinated metal sites bind to the CO 2 RR intermediates more weakly.…”

Section: Co 2 To Comentioning

confidence: 99%