Chemoenzymatic Photoreforming: A Sustainable Approach for Solar Fuel Generation from Plastic Feedstocks.

Chemoenzymatic Photoreforming: A Sustainable Approach for Solar Fuel Generation from Plastic Feedstocks.
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化学酶照明形成:塑料原料产生太阳能燃料的可持续方法。

DOI:
10.1021/jacs.3c05486
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发表时间:
2023-09-20
影响因子:
15
通讯作者:
Reisner, Erwin
Reisner, Erwin
中科院分区:
化学1区
文献类型:
--
作者:
Bhattacharjee, Subhajit;Guo, Chengzhi;Lam, Erwin;Holstein, Josephin M.;Rangel Pereira, Mariana;Pichler, Christian M.;Pornrungroj, Chanon;Rahaman, Motiar;Uekert, Taylor;Hollfelder, Florian;Reisner, Erwin

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通过催化转化的塑料升级回收是一个有吸引力的废物增值概念,但从塑料中清洁和节能地生产高价值产品仍然具有挑战性。在这里,我们介绍了化学酶光重整作为一种将酶预处理和太阳能驱动的聚酯塑料重整相结合的工艺,在温和的温度和pH下生产清洁的H2和增值化学品。化学酶光重整在聚酯薄膜和纳米塑料的升级循环中显示出多用途性,以高达103-104 μmol gcat-1的高产率和>500 μmol gcat-1 h-1的活性生产H2。酶处理的塑料也被用作电子供体,用于光催化二氧化碳到合成气的转化,并与固定在TiO2纳米颗粒(TiO2|CotpyP)上的磷酸钴二(三联吡啶)催化剂相结合。最后,技术经济分析表明,化学酶光重整方法有可能大幅降低氢气生产成本,与化石燃料生产氢气的市场价格相当,同时保持较低的二氧化碳当量排放。
Plastic upcycling through catalytic transformations is an attractive concept to valorize waste, but the clean and energy-efficient production of high-value products from plastics remains challenging. Here, we introduce chemoenzymatic photoreforming as a process coupling enzymatic pretreatment and solar-driven reforming of polyester plastics under mild temperatures and pH to produce clean H2 and value-added chemicals. Chemoenzymatic photoreforming demonstrates versatility in upcycling polyester films and nanoplastics to produce H2 at high yields reaching ∼103–104 μmol gsub–1 and activities at >500 μmol gcat–1 h–1. Enzyme-treated plastics were also used as electron donors for photocatalytic CO2-to-syngas conversion with a phosphonated cobalt bis(terpyridine) catalyst immobilized on TiO2 nanoparticles (TiO2|CotpyP). Finally, techno-economic analyses reveal that the chemoenzymatic photoreforming approach has the potential to drastically reduce H2 production costs to levels comparable to market prices of H2 produced from fossil fuels while maintaining low CO2-equivalent emissions.
DOI: 10.1126/sciadv.1700782
发表时间: 2017-07
期刊: Science advances
影响因子: 13.6
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DOI: 10.1007/bf02083881
发表时间: 1996-01-01
期刊: JOURNAL OF ENVIRONMENTAL POLYMER DEGRADATION
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