Carbon nitride-TiO(2) hybrid modified with hydrogenase for visible light driven hydrogen production.

Carbon nitride-TiO(2) hybrid modified with hydrogenase for visible light driven hydrogen production.
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DOI:
10.1039/c5sc02017d
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发表时间:
2015-10-01
期刊:
影响因子:
8.4
通讯作者:
Reisner E
Reisner E
中科院分区:
化学1区
文献类型:
--
作者:
Caputo CA;Wang L;Beranek R;Reisner E

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据报道,在氮化碳-TiO2 混合物上使用异质化氢化酶进行太阳能驱动的氢气生产,为光制氢树立了新的基准。报道了一种由[NiFeSe]-氢化酶(H2ase)组成的系统,该系统接枝在用聚庚嗪碳氮化物聚合物瓜(CNx)改性的TiO2纳米颗粒的表面。在太阳 AM 1.5 G 照射期间,在 pH 6 的牺牲电子供体溶液中 72 小时后,该半生物组装体的周转数 (TON) 超过 5.8 × 105 mol H2 (mol H2ase)–1。在单色光照射下,光子-氢转换的外量子效率高达4.8%。 CNx-TiO2-H2ase 结构在无紫外线的太阳光照射下(λ > 420 nm)也具有活性,其活性明显高于 TiO2-H2ase 和 CNx-H2ase,部分原因是 CNx-TiO2 电荷转移复合物的形成以及向 H2ase 的高产电子转移。 CNx-TiO2-H2ase 系统在可见光利用率和稳定性方面为光催化制氢树立了新的基准,该系统将 H2ase 固定在不含贵金属和有毒金属的光吸收剂上。
Solar light driven hydrogen production with a heterogenised hydrogenase on a carbon nitride–TiO2 hybrid is reported that sets a new benchmark for photo-H2 production. A system consisting of a [NiFeSe]–hydrogenase (H2ase) grafted on the surface of a TiO2 nanoparticle modified with polyheptazine carbon nitride polymer, melon (CNx) is reported. This semi-biological assembly shows a turnover number (TON) of more than 5.8 × 105 mol H2 (mol H2ase)–1 after 72 h in a sacrificial electron donor solution at pH 6 during solar AM 1.5 G irradiation. An external quantum efficiency up to 4.8% for photon-to-hydrogen conversion was achieved under irradiation with monochromatic light. The CNx–TiO2–H2ase construct was also active under UV-free solar light irradiation (λ > 420 nm), where it showed a substantially higher activity than TiO2–H2ase and CNx–H2ase due, in part, to the formation of a CNx–TiO2 charge transfer complex and highly productive electron transfer to the H2ase. The CNx–TiO2–H2ase system sets a new benchmark for photocatalytic H2 production with a H2ase immobilised on a noble- and toxic-metal free light absorber in terms of visible light utilisation and stability.
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