Nanowire-bacteria hybrids for unassisted solar carbon dioxide fixation to value-added chemicals.
Nanowire-bacteria hybrids for unassisted solar carbon dioxide fixation to value-added chemicals.
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DOI：
10.1021/acs.nanolett.5b01254
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发表时间：
2015-05-13
期刊：
影响因子：
10.8
通讯作者：
Yang P
中科院分区：
文献类型：
--
作者：
Liu C;Gallagher JJ;Sakimoto KK;Nichols EM;Chang CJ;Chang MC;Yang P
利用太阳能直接利用二氧化碳和水生产增值化学品是一种模仿自然光合作用的过程，具有重要的基础和实际意义。在自然光合作用中，二氧化碳首先利用太阳能被还原为常见的生化构件，随后用于合成形成生物质的分子产物的复杂混合物。在这里，我们报告了一种人工光合作用方案，该方案通过开发生物相容性的光捕获纳米线阵列来通过类似的两步过程发挥作用，该阵列能够与微生物系统直接接口。作为原理证明，我们证明混合半导体纳米线-细菌系统可以仅使用太阳能输入，在中性 pH 值下将二氧化碳还原到各种化学目标，例如燃料、聚合物和复杂的药物前体。高表面积硅纳米线阵列收集光能，为厌氧细菌卵形孢子菌提供还原当量，用于在有氧条件（21% O2）下光电化学生产乙酸，具有低过电位（η < 200 mV）、高法拉第效率（高达 90%）和长期稳定性（长达 200 小时）。所得乙酸盐（约 6 g/L）可被基因工程大肠杆菌激活为乙酰辅酶 A (乙酰-CoA)，并可用作各种增值化学品的构建模块，例如正丁醇、聚羟基丁酸酯 (PHB) 聚合物和三种不同的类异戊二烯天然产物。因此，将生物相容性固态纳米器件与生命系统连接起来，为开发完全由阳光驱动的可编程化学合成系统提供了一个起点。
Direct solar-powered production of value-added chemicals from CO2 and H2O, a process that mimics natural photosynthesis, is of fundamental and practical interest. In natural photosynthesis, CO2 is first reduced to common biochemical building blocks using solar energy, which are subsequently used for the synthesis of the complex mixture of molecular products that form biomass. Here we report an artificial photosynthetic scheme that functions via a similar two-step process by developing a biocompatible light-capturing nanowire array that enables a direct interface with microbial systems. As a proof of principle, we demonstrate that a hybrid semiconductor nanowire-bacteria system can reduce CO2 at neutral pH to a wide array of chemical targets, such as fuels, polymers, and complex pharmaceutical precursors, using only solar energy input. The high surface-area silicon nanowire array harvests light energy to provide reducing equivalents to the anaerobic bacterium, Sporomusa ovata, for the photoelectrochemical production of acetic acid under aerobic conditions (21% O2) with low overpotential (η < 200 mV), high Faradic efficiency (up to 90%), and long-term stability (up to 200 hours). The resulting acetate (~ 6 g/L) can be activated to acetyl coenzyme A (acetyl-CoA) by genetically engineered Escherichia coli and used as a building block for a variety of value-added chemicals, such as n-butanol, polyhydroxybutyrate (PHB) polymer, and three different isoprenoid natural products. As such, interfacing biocompatible solid-state nanodevices with living systems provides a starting point for developing a programmable system of chemical synthesis entirely powered by sunlight.
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