Understanding Structure-Activity Relationship in Pt-loaded g-C3N4 for Efficient Solar- Photoreforming of Polyethylene Terephthalate Plastic and Hydrogen Production,Small Methods

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Understanding Structure-Activity Relationship in Pt-loaded g-C3N4 for Efficient Solar- Photoreforming of Polyethylene Terephthalate Plastic and Hydrogen Production
Small Methods ( IF 10.7 ) Pub Date : 2023-09-15 , DOI: 10.1002/smtd.202300427
Thi Kim Anh Nguyen _{1,

2} , Thành Trần-Phú _{1,

2} , Xuan Minh Chau Ta _{1,

2} , Thien N Truong ₃ , Josh Leverett ₄ , Rahman Daiyan ₄ , Rose Amal ₄ , Antonio Tricoli _{1,

2}

Affiliation

Coupling the hydrogen evolution reaction with plastic waste photoreforming provides a synergistic path for simultaneous production of green hydrogen and recycling of post-consumer products, two major enablers for establishment of a circular economy. Graphitic carbon nitride (g-C₃N₄) is a promising photocatalyst due to its suitable optoelectronic and physicochemical properties, and inexpensive fabrication. Herein, a mechanistic investigation of the structure-activity relationship of g-C₃N₄ for poly(ethylene terephthalate) (PET) photoreforming is reported by carefully controlling its fabrication from a subset of earth-abundant precursors, such as dicyandiamide, melamine, urea, and thiourea. These findings reveal that melamine-derived g-C₃N₄ with 3 wt.% Pt has significantly higher performance than alternative derivations, achieving a maximum hydrogen evolution rate of 7.33 mmol_H2 g_cat⁻¹ h⁻¹, and simultaneously photoconverting PET into valuable organic products including formate, glyoxal, and acetate, with excellent stability for over 30 h of continuous production. This is attributed to the higher crystallinity and associated chemical resistance of melamine-derived g-C₃N₄, playing a major role in stabilization of its morphology and surface properties. These new insights on the role of precursors and structural properties in dictating the photoactivity of g-C₃N₄ set the foundation for the further development of photocatalytic processes for combined green hydrogen production and plastic waste reforming.

中文翻译：

了解负载 Pt 的 g-C3N4 的构效关系，以实现聚对苯二甲酸乙二醇酯塑料的高效太阳能光重整和氢气生产

将析氢反应与塑料废物光重整相结合，为同时生产绿色氢气和回收消费后产品提供了一条协同途径，这是建立循环经济的两个主要推动力。石墨氮化碳（ g -C ₃ N ₄ ）由于其合适的光电和物理化学性质以及廉价的制造而成为一种有前途的光催化剂。在此，通过仔细控制来自地球丰富_的前体子集（例如_双氰胺、三聚氰胺、尿素和硫脲。这些发现表明，含有 3 wt.% Pt 的三聚氰胺衍生的g -C ₃ N ₄具有比其他衍生产品显着更高的性能，实现了 7.33 mmol _H2 g _cat ^-1 h ^-1的最大析氢速率，并同时将 PET 光转化为有价值的有机产品，包括甲酸盐、乙二醛和乙酸盐，在连续生产超过 30 小时时具有出色的稳定性。这归因于三聚氰胺衍生的g -C ₃ N ₄具有较高的结晶度和相关的耐化学性，在稳定其形态和表面性质方面发挥着重要作用。这些关于前驱体的作用和结构特性在决定g -C ₃ N ₄光活性方面的新见解为进一步开发绿色氢生产和塑料废物重整相结合的光催化工艺奠定了基础。

更新日期：2023-09-15

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