Structurally Diverse Covalent Triazine-Based Framework Materials for Photocatalytic Hydrogen Evolution from Water

Structurally Diverse Covalent Triazine-Based Framework Materials for Photocatalytic Hydrogen Evolution from Water
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DOI:
10.1021/acs.chemmater.9b02825
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发表时间:
2019-11-12
影响因子:
8.6
通讯作者:
Cooper, Andrew I.
Cooper, Andrew I.
中科院分区:
材料科学2区
文献类型:
--
作者:
Meier, Christian B.;Clowes, Rob;Cooper, Andrew I.

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通过Suzuki-Miyaura缩聚合成了一个结构多样的39种共价三嗪基框架材料(CTF)家族,并使用高通量工作流程作为析氢光催化剂进行了测试。这两种性能最好的CTF分别基于苄腈和二苯并[B,d]噻吩砜连接体,其催化活性在该材料类别中最高。不同的CTF的活动是合理化的四个变量:预测的电子亲和势,预测的电离势,光学间隙,并在溶液中的CTF颗粒,如通过光学透射率测量的电子密度。结果表明,溶液中的电子亲合势和pH值是光催化析氢活性的最佳预测因子。
A structurally diverse family of 39 covalent triazine-based framework materials (CTFs) are synthesized by Suzuki-Miyaura polycondensation and tested as hydrogen evolution photocatalysts using a high-throughput workflow. The two best-performing CTFs are based on benzonitrile and dibenzo[b,d]thiophene sulfone linkers, respectively, with catalytic activities that are among the highest for this material class. The activities of the different CTFs are rationalized in terms of four variables: the predicted electron affinity, the predicted ionization potential, the optical gap, and the dispersibility of the CTFs particles in solution, as measured by optical transmittance. The electron affinity and dispersibility in solution are found to be the best predictors of photocatalytic hydrogen evolution activity.