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首页> 外文期刊>Catalysis science & technology >Regulating morphological and electronic structures of polymeric carbon nitrides by successive copolymerization and stream reforming for photocatalytic CO2 reduction
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Regulating morphological and electronic structures of polymeric carbon nitrides by successive copolymerization and stream reforming for photocatalytic CO2 reduction

机译：调节形态和电子结构连续聚合碳氮化物共聚和流改革二氧化碳光催化还原

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摘要

Polymeric carbon nitrides (PCNs) are attractive candidates for diverse photoredox catalysis, but the CO2 reduction activity of pristine PCNs is unsatisfactory, mainly due to the bulky structure and insufficient optical harvesting. In this work, a facile and efficient strategy coupling copolymerization and stream reforming is developed to exfoliate the bulky PCNs into PCN nanosheets (named PCN-T-NSs). The ameliorated morphological and electronic structures of PCN-T-NSs enable the exposure of abundant catalytically-active sites, accelerated separation of photogenerated charge carriers, and strengthened photoabsorption in the visible region. Consequently, the optimized PCN-T-NS photocatalyst shows a greatly enhanced CO2 reduction activity, with a remarkable CO-releasing rate of 43 mu mol h(-1), which is about 40 times greater than that of pristine PCN. Besides, a high apparent quantum efficiency (AQE) of 4.2% is realized by the PCN-T-NS catalyst under 420 nm photoirradiation with TEOA as a sacrificial reagent and Co(bpy)(3)(2+) as a cocatalyst. Moreover, the integrated copolymerization and stream reforming strategy is extendable to the assembly of several other carbon nitride nanosheets with enhanced performance for CO2 photoreduction by employing the typical comonomers. This work may bring some fresh vitality for constructing well-tailored carbon nitride polymers with functions for sustainable solar-to-chemical energy conversion.
机译：高分子碳氮化物(PCNs)有吸引力候选人不同photoredox催化,但是二氧化碳减排活动的原始PCNs不满意,主要是由于庞大的结构和光学收获不足。工作,一个简单和有效的战略耦合共聚和流改革去角质笨重PCNs成PCN开发的nanosheets(名为PCN-T-NSs)。形态和电子结构PCN-T-NSs使丰富的接触catalytically-active网站,加速photogenerated载流子的分离加强在可见的光吸收地区。光催化剂显示了极大地增强了二氧化碳减少活动,引人注目CO-releasing 43亩摩尔h(1),这是约40倍的原始PCN。此外,表观量子效率高(AQE)PCN-T-NS实现4.2%的催化剂在420纳米和TEOA作为光致辐照牺牲试剂和Co (bpy) (3) (2 +)助催化剂。共聚和流改革策略其他的可扩展到组装氮化碳nanosheets与增强采用二氧化碳性能的光致还原作用典型的共聚单体。剪裁精良构造新鲜活力碳氮化与功能聚合物可持续solar-to-chemical能源转换。

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