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Photoenzymatic Catalytic Cascade System of a Pyromellitic Diimide/g-C3N4 Heterojunction to Efficiently Regenerate NADH for Highly Selective CO2 Reduction toward Formic Acid
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2021-09-23 , DOI: 10.1021/acsami.1c13167 Pengye Zhang 1 , Jundie Hu 2 , Yangbin Shen 2 , Xiaogang Yang 2 , Jiafu Qu 2 , Feng Du 2 , Wei Sun 3 , Chang Ming Li 1, 2, 3, 4
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2021-09-23 , DOI: 10.1021/acsami.1c13167 Pengye Zhang 1 , Jundie Hu 2 , Yangbin Shen 2 , Xiaogang Yang 2 , Jiafu Qu 2 , Feng Du 2 , Wei Sun 3 , Chang Ming Li 1, 2, 3, 4
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Photocatalytic reduction of carbon dioxide (CO2) holds great promise for both clean energy and environment protection. However, the low activity and poor selectivity of photocatalysts are the main bottlenecks. Herein, inspired by artificial photosynthesis and taking advantages of high efficiency and specificity of bioenzymes, we marry photo with enzyme to synergistically solve the above problems. A metal-free heterojunction of pyromellitic diimide/g-C3N4 (PDI/CN) with an excellent visible light response (λ < 660 nm) is fabricated for achieving a photoenzymatic catalytic cascade system, which efficiently regenerates nicotinamide adenine dinucleotide (NADH) and selectively reduces CO2 to formic acid (HCOOH). The highest NADH yield of the PDI/CN hybrid achieved is 75%, and the HCOOH generation rate achieved is 1.269 mmol g–1 h–1 with nearly 100% selectivity, which is much higher than those of the reported materials. The excellent photocatalytic performance is attributed to the unique photoenzymatic catalytic cascade system, heterointerface effect, good conductivity, and a wide sunlight response range of the PDI/CN heterojunction. This work provides an efficient strategy and a corresponding photocatalyst for the directional conversion of CO2 to HCOOH.
中文翻译：
均苯四甲酸二亚胺/g-C3N4 异质结的光酶催化级联系统可有效再生 NADH 以实现对甲酸的高选择性 CO2 还原
二氧化碳 (CO 2 ) 的光催化还原对于清洁能源和环境保护具有广阔的前景。然而，光催化剂的低活性和选择性差是主要的瓶颈。在此，我们受人工光合作用的启发，利用生物酶的高效性和特异性，将光与酶结合，协同解决上述问题。制备了具有优异可见光响应 (λ < 660 nm)的均苯四甲酸二亚胺/gC 3 N 4 (PDI/CN)的无金属异质结，用于实现光酶催化级联系统，该系统可有效再生烟酰胺腺嘌呤二核苷酸 (NADH) 和选择性还原 CO 2到甲酸 (HCOOH)。PDI/CN 杂化物的最高 NADH 产率为 75%，HCOOH 生成率为 1.269 mmol g –1 h –1，选择性接近 100%，远高于报道的材料。优异的光催化性能归功于PDI/CN异质结独特的光酶催化级联系统、异质界面效应、良好的导电性和较宽的阳光响应范围。这项工作为CO 2定向转化为HCOOH提供了一种有效的策略和相应的光催化剂。
更新日期：2021-10-06
中文翻译：
均苯四甲酸二亚胺/g-C3N4 异质结的光酶催化级联系统可有效再生 NADH 以实现对甲酸的高选择性 CO2 还原
二氧化碳 (CO 2 ) 的光催化还原对于清洁能源和环境保护具有广阔的前景。然而，光催化剂的低活性和选择性差是主要的瓶颈。在此，我们受人工光合作用的启发，利用生物酶的高效性和特异性，将光与酶结合，协同解决上述问题。制备了具有优异可见光响应 (λ < 660 nm)的均苯四甲酸二亚胺/gC 3 N 4 (PDI/CN)的无金属异质结，用于实现光酶催化级联系统，该系统可有效再生烟酰胺腺嘌呤二核苷酸 (NADH) 和选择性还原 CO 2到甲酸 (HCOOH)。PDI/CN 杂化物的最高 NADH 产率为 75%，HCOOH 生成率为 1.269 mmol g –1 h –1，选择性接近 100%，远高于报道的材料。优异的光催化性能归功于PDI/CN异质结独特的光酶催化级联系统、异质界面效应、良好的导电性和较宽的阳光响应范围。这项工作为CO 2定向转化为HCOOH提供了一种有效的策略和相应的光催化剂。
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