Molecular Trade-Offs between Lattice Oxygen and Oxygen Vacancy Drive Organic Pollutant Degradation in Fungal Biomineralized Exoskeletons

Molecular Trade-Offs between Lattice Oxygen and Oxygen Vacancy Drive Organic Pollutant Degradation in Fungal Biomineralized Exoskeletons
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晶格氧和氧空位之间的分子权衡驱动真菌生物矿化外骨骼有机污染物降解

DOI:
10.1021/acs.est.2c01388
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发表时间:
2022-06-21
影响因子:
11.4
通讯作者:
Gadd, Geoffrey Michael
Gadd, Geoffrey Michael
中科院分区:
环境科学与生态学1区
文献类型:
--
作者:
Chi, Zhi-Lai;Yu, Guang-Hui;Gadd, Geoffrey Michael

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真菌-矿物相互作用可有效缓解有机污染物对细胞造成的压力,由于地球进入前所未有的地质时代-人类世,预计有机污染物的产生将迅速增加。在真菌-矿物相互作用过程中,可能使真菌能够对抗有机污染的潜在机制仍不清楚。受自然真菌孢子形成过程的启发,我们首次证明真菌生物矿化触发菌丝上富含纳米级铁(oxyhydr)氧化物和生物分子的外骨骼(数百纳米厚)的形成。通过高空间分辨率(低至50 nm)的同步辐射技术,在亚细胞尺度上绘制了该涂层的生化组成,证实了芳香族C,C-N键,酰胺羰基和铁(羟基)氧化物作为涂层的主要成分。这种纳米生物杂化系统似乎通过改变晶格氧和氧空位之间的分子水平的权衡,赋予双酚A的真菌降解强(x2)的生物功能性。真菌涂层可以作为“人造孢子”,使真菌能够对抗自然环境中的物理和化学应力,为真菌生物矿化和地球岩石圈和生物圈的共同进化提供重要见解。
Fungal-mineral interactions can effectively alleviate cellular stress from organic pollutants, the production of which are expected to rapidly increase owing to the Earth moving into an unprecedented geological epoch, the Anthropocene. The underlying mechanisms that may enable fungi to combat organic pollution during fungal-mineral interactions remain unclear. Inspired by the natural fungal sporulation process, we demonstrate for the first time that fungal biomineralization triggers the formation of an ultrathin (hundreds of nanometers thick) exoskeleton, enriched in nanosized iron (oxyhydr)oxides and biomolecules, on the hyphae. Mapped biochemical composition of this coating at a subcellular scale via high spatial resolution (down to 50 nm) synchrotron radiation-based techniques confirmed aromatic C, C-N bonds, amide carbonyl, and iron (oxyhydr)oxides as the major components of the coatings. This nanobiohybrid system appeared to impart a strong (x2) biofunctionality for fungal degradation of bisphenol A through altering molecular-level trade-offs between lattice oxygen and oxygen vacancy. Together, fungal coatings could act as "artificial spores", which enable fungi to combat physical and chemical stresses in natural environments, providing crucial insights into fungal biomineralization and coevolution of the Earth's lithosphere and biosphere.