Photosynthetic biohybrid coculture for tandem and tunable CO(2) and N(2) fixation.

Photosynthetic biohybrid coculture for tandem and tunable CO(2) and N(2) fixation.
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DOI:
10.1073/pnas.2122364119
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发表时间:
2022-06-28
影响因子:
11.1
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中科院分区:
综合性期刊1区
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将(光)电化学平台与作为“活”生物催化剂的CO2固定细菌相结合,实现了将CO2高度选择性地还原为C2+产物,如乙酸盐。这种方法还能够将初始CO2产品下游转化为更高价值的产品。我们报告了这一概念的进展,通过共培养初级CO2固定细菌生产乙酸与二级N2固定细菌,采用乙酸减少N2到NH3,并产生生物塑料。共生共培养物可以电化学控制和模块化调节以产生所需的产物流。我们预计,该平台可以扩展到仅从CO2,N2,H2O和电力生产其他几种产品,包括生物塑料,生物燃料和糖。太阳能驱动的生物电合成是一种很有前途的方法,可以将丰富的资源转化为具有可再生能源的增值化学品。由电化学还原当量提供动力的微生物同化CO2、H2O和N2构建块。然而,来自自养全细胞生物催化剂的产物是有限的。此外,生物催化剂的任务与N2还原的限制,同时能源密集型自养。为了克服这些挑战,我们设计了一种生物混合共培养物,用于串联和可调的CO2和N2固定到增值产品,允许不同的物种分布生物转化步骤并减少个体代谢负担。该财团涉及产乙酸菌Sporomusa ovata,其将CO2还原为乙酸盐,和重氮营养型Rhodopyramidpalustris,其使用乙酸盐来燃料N2固定和用于产生生物聚酯。我们证明,共培养平台提供了一个强大的生态系统,连续CO2和N2固定,其输出是由底物气体组成。此外,我们显示出支持在高表面积硅纳米线阴极平台上共培养的能力。生物杂交共培养实现了100,19.1,和6.3%的峰值法拉第效率的乙酸,生物质中的氮,和氨,分别,同时保持产品的可调性。最后,我们建立了由光伏装置驱动的完全太阳能到化学转化,导致乙酸盐、含氮生物质和氨的太阳能到化学效率分别为1.78%、0.51%和0.08%。最终,我们的工作证明了根据需要使用和电化学操纵细菌群落以扩大CO2和N2生物电合成产品套件的能力。
Combining (photo)electrochemical platforms with CO2 -fixing bacteria as “living” biocatalysts has realized the highly selective reduction of CO2 to C2+ products, such as acetate. This approach also enables the downstream conversion of the initial CO2 product to a higher-value one. We report an advance on this concept by coculturing primary CO2-fixing bacteria producing acetate with secondary N2-fixing bacteria that employ the acetate to reduce N2 to NH3 and to generate a bioplastic. The symbiotic coculture can be controlled electrochemically and modularly tuned to generate a desired product stream. We foresee that this platform could be expanded to produce several additional products, including bioplastics, biofuels, and sugars, from only CO2, N2, H2O, and electricity. Solar-driven bioelectrosynthesis represents a promising approach for converting abundant resources into value-added chemicals with renewable energy. Microorganisms powered by electrochemical reducing equivalents assimilate CO2, H2O, and N2 building blocks. However, products from autotrophic whole-cell biocatalysts are limited. Furthermore, biocatalysts tasked with N2 reduction are constrained by simultaneous energy-intensive autotrophy. To overcome these challenges, we designed a biohybrid coculture for tandem and tunable CO2 and N2 fixation to value-added products, allowing the different species to distribute bioconversion steps and reduce the individual metabolic burden. This consortium involves acetogen Sporomusa ovata, which reduces CO2 to acetate, and diazotrophic Rhodopseudomonas palustris, which uses the acetate both to fuel N2 fixation and for the generation of a biopolyester. We demonstrate that the coculture platform provides a robust ecosystem for continuous CO2 and N2 fixation, and its outputs are directed by substrate gas composition. Moreover, we show the ability to support the coculture on a high–surface area silicon nanowire cathodic platform. The biohybrid coculture achieved peak faradaic efficiencies of 100, 19.1, and 6.3% for acetate, nitrogen in biomass, and ammonia, respectively, while maintaining product tunability. Finally, we established full solar to chemical conversion driven by a photovoltaic device, resulting in solar to chemical efficiencies of 1.78, 0.51, and 0.08% for acetate, nitrogenous biomass, and ammonia, correspondingly. Ultimately, our work demonstrates the ability to employ and electrochemically manipulate bacterial communities on demand to expand the suite of CO2 and N2 bioelectrosynthesis products.
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