Catalytically potent and selective clusterzymes for modulation of neuroinflammation through single-atom substitutions.
Catalytically potent and selective clusterzymes for modulation of neuroinflammation through single-atom substitutions.
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通过单原子取代调节神经炎症的催化有效和选择性簇酶
DOI：
10.1038/s41467-020-20275-0
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发表时间：
2021-01-07
影响因子：
16.6
通讯作者：
Zhang XD
中科院分区：
文献类型：
--
作者：
Liu H;Li Y;Sun S;Xin Q;Liu S;Mu X;Yuan X;Chen K;Wang H;Varga K;Mi W;Yang J;Zhang XD
具有重编程和增强的催化活性和底物选择性的新兴人工酶长期以来一直在持续努力。与天然分子相比，目前大多数候选分子的催化活性相当差。为了解决这一限制，我们设计了人工酶的基础上，结构上定义良好的Au 25簇，即clusterzymes，这是具有内在的高催化活性和选择性驱动的单原子取代调制键长。Au 24 Cu 1和Au 24 Cd 1簇合酶的抗氧化能力分别是天然Trolox的137倍和160倍。同时，簇合酶表现出优先的酶模拟催化活性，与Au 25，Au 24 Cu 1和Au 24 Cd 1显示令人信服的选择性谷胱甘肽过氧化物酶样（GPx-样），过氧化氢酶样（CAT-样）和超氧化物歧化酶样（SOD-样）的活动，分别。Au 24 Cu 1通过催化反应减少损伤脑中的过氧化物，而Au 24 Cd 1优先使用超氧化物和含氮信号分子作为底物，并显著减少炎症因子，表明在减轻神经炎症中的重要作用。具有重编程和增强的催化活性和底物选择性的人工酶已经出现，以解决贵金属或过渡金属氧化物的限制。在这里，作者报道了在一系列酶模拟反应中具有高催化活性和选择性的Au 25簇合酶。
Emerging artificial enzymes with reprogrammed and augmented catalytic activity and substrate selectivity have long been pursued with sustained efforts. The majority of current candidates have rather poor catalytic activity compared with natural molecules. To tackle this limitation, we design artificial enzymes based on a structurally well-defined Au25 cluster, namely clusterzymes, which are endowed with intrinsic high catalytic activity and selectivity driven by single-atom substitutions with modulated bond lengths. Au24Cu1 and Au24Cd1 clusterzymes exhibit 137 and 160 times higher antioxidant capacities than natural trolox, respectively. Meanwhile, the clusterzymes demonstrate preferential enzyme-mimicking catalytic activities, with Au25, Au24Cu1 and Au24Cd1 displaying compelling selectivity in glutathione peroxidase-like (GPx-like), catalase-like (CAT-like) and superoxide dismutase-like (SOD-like) activities, respectively. Au24Cu1 decreases peroxide in injured brain via catalytic reactions, while Au24Cd1 preferentially uses superoxide and nitrogenous signal molecules as substrates, and significantly decreases inflammation factors, indicative of an important role in mitigating neuroinflammation. Artificial enzymes with reprogrammed and augmented catalytic activity and substrate selectivity have emerged to tackle limitations of noble metals or transition metal oxides. Here, the authors report Au25 clusterzymes which are endowed with high catalytic activity and selectivity in a range of enzyme-mimicking reactions.
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影响因子：
16.6
作者：
Imaoka T;Akanuma Y;Haruta N;Tsuchiya S;Ishihara K;Okayasu T;Chun WJ;Takahashi M;Yamamoto K
通讯作者：
Yamamoto K
影响因子：
38.3
作者：
Jiang, Xingya;Du, Bujie;Zheng, Jie
通讯作者：
Zheng, Jie
影响因子：
17.1
作者：
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通讯作者：
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通过纳米催化剂递送，肿瘤选择性催化纳米医学。
影响因子：
16.6
作者：
Huo M;Wang L;Chen Y;Shi J
通讯作者：
Shi J
多种纳米酶的自组装模拟细胞内抗氧化防御系统
影响因子：
16.6
作者：
Huang, Yanyan;Liu, Zhen;Qu, Xiaogang
通讯作者：
Qu, Xiaogang