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2D photosensitive porphyrin-based MOFs integrated with a Pd cocatalyst with fast charge transfer for efficient photocatalytic hydrogen evolution
Catalysis Science & Technology ( IF 4.4 ) Pub Date : 2023-08-04 , DOI: 10.1039/d3cy00705g Yacen Tang 1 , Mingzuo Chen 1 , Chenghua Zhang 2 , Huyumao Li 1 , Youzhou He 1 , Xiangdong Lai 3 , Liujun Tao 1 , Jiajia Jing 1 , Xingyan Liu 1
Catalysis Science & Technology ( IF 4.4 ) Pub Date : 2023-08-04 , DOI: 10.1039/d3cy00705g Yacen Tang 1 , Mingzuo Chen 1 , Chenghua Zhang 2 , Huyumao Li 1 , Youzhou He 1 , Xiangdong Lai 3 , Liujun Tao 1 , Jiajia Jing 1 , Xingyan Liu 1
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To improve the charge carrier transport efficiency via reducing the transmission distance, a series of 2D MOF nanosheets with several transition metal clusters as metal nodes are prepared by a simple hydrothermal method for photocatalytic hydrogen production, in which PdTCPP integrates a photosensitive porphyrin with cocatalysts so as to realize fast charge carrier transport. The experimental results show that Co–TCPP(Pd) has the most outstanding hydrogen evolution activity (4.40 mmol g−1 h−1), which could be the reason that the noble metal Pd anchored in the porphyrin center plays a significant role in the electron transfer process, that is, the photogenerated electrons generated by the multivalent Co-oxo cluster excited by illumination are transferred from its own LUMO energy level to the self-photosensitized porphyrin ring through –COO–, and then together transferred to the active site of the precious metal Pd in the porphyrin center to achieve effective hydrogen evolution. The results provide us a feasible strategy to integrate the individual photosensitive porphyrin center with the cocatalysts into sole metalloporphyrins so as to shorten the charge carrier transmission distance for ultimately further improving the photocatalytic performance.
中文翻译：
二维光敏卟啉基 MOF 与 Pd 助催化剂集成，具有快速电荷转移功能，可实现高效光催化析氢
为了通过减少传输距离来提高载流子传输效率，通过简单的水热法制备了一系列以多个过渡金属簇作为金属节点的二维MOF纳米片用于光催化制氢，其中PdTCPP将光敏卟啉与助催化剂结合在一起，从而实现载流子的快速传输。实验结果表明Co-TCPP(Pd)具有最突出的析氢活性(4.40 mmol g −1 h −1），这可能是锚定在卟啉中心的贵金属Pd在电子转移过程中发挥重要作用的原因，即多价Co-oxo簇在光照激发下产生的光生电子从其自身的LUMO转移能级通过-COO-转移到自光敏化的卟啉环上，然后一起转移到卟啉中心的贵金属Pd的活性位点，实现有效的析氢。研究结果为我们提供了一种可行的策略，将单个光敏卟啉中心与助催化剂整合成单一金属卟啉，以缩短载流子传输距离，最终进一步提高光催化性能。
更新日期：2023-08-04
中文翻译：
二维光敏卟啉基 MOF 与 Pd 助催化剂集成，具有快速电荷转移功能，可实现高效光催化析氢
为了通过减少传输距离来提高载流子传输效率，通过简单的水热法制备了一系列以多个过渡金属簇作为金属节点的二维MOF纳米片用于光催化制氢，其中PdTCPP将光敏卟啉与助催化剂结合在一起，从而实现载流子的快速传输。实验结果表明Co-TCPP(Pd)具有最突出的析氢活性(4.40 mmol g −1 h −1），这可能是锚定在卟啉中心的贵金属Pd在电子转移过程中发挥重要作用的原因，即多价Co-oxo簇在光照激发下产生的光生电子从其自身的LUMO转移能级通过-COO-转移到自光敏化的卟啉环上，然后一起转移到卟啉中心的贵金属Pd的活性位点，实现有效的析氢。研究结果为我们提供了一种可行的策略，将单个光敏卟啉中心与助催化剂整合成单一金属卟啉，以缩短载流子传输距离，最终进一步提高光催化性能。
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