Developing efficient,stable and sustainable photocatalysts for water splitting is one of the most significant methods for generating hydrogen.Conjugated microporous polymers,as a new type of organic semiconductor phot...Developing efficient,stable and sustainable photocatalysts for water splitting is one of the most significant methods for generating hydrogen.Conjugated microporous polymers,as a new type of organic semiconductor photocatalyst,have adjustable bandgaps and high specific surface areas,and can be synthesized using diverse methods.In this work,we report the design and synthesis of a series of pyridyl conjugated microporous polymers(PCMPs)utilizing polycondensation of aromatic aldehydes and aromatic ketones in the presence of ammonium acetate.PCMPs with different chemical structures were synthesized via adjusting monomers with different geometries and contents of nitrogen element,which could adjust the bandgap and photocatalytic performance.Photocatalytic hydrogen evolution rate(HER)up to 1198.9μmol·h^(-1)·g^(-1) was achieved on the optimized polymer with a specific surface area of 312 m^(2)·g^(-1) under UV-Vis light irradiation(A>320 nm).This metal-free synthetic method provides a new avenue to preparing an efficient photocatalyst for hydrogen evolution.展开更多
The development of trimethylamine (TMA) gassensors is crucial for environmental monitoring, food safety,and health surveillance. However, it is difficult to achievestable detection of TMA with low concentration at a l...The development of trimethylamine (TMA) gassensors is crucial for environmental monitoring, food safety,and health surveillance. However, it is difficult to achievestable detection of TMA with low concentration at a lowtemperature. In this work, a series of conjugated microporouspolytriphenylamine (PTPA) were designed and synthesized,with tunable porosity and surface area, using Hansen solubilityparameters and nanosilica spheres as templates. Comparedto pure PTPA (R = 4 for 100 ppm), the modified PTPAderivatives exhibited significantly enhanced TMA sensingperformance, with NaF-PTPA achieving a remarkable sensitivity(R = 22 for 100 ppm) and a low detection limit of0.53 ppm. The NaF-PTPA based sensor also demonstratedexcellent long-term stability, maintaining consistent performanceover 30 days at 54 °C. The impressive results can beattributed to the protonation (–NH_(2)^(+)), modified porosity andincreased surface area. Hence, this strategy presents new insightsfor the advancement of low-temperature sensing technologies.展开更多
基金the National Natural Science Foundation of China(Nos.52073046,51873036 and 51673039)the Chang Jiang Scholars Program(No.Q2019152)+4 种基金the Fundamental Research Funds for the Central Universities(No.2232019A3-01)the Shanghai Shuguang Program(No.19SG28)the Shanghai Natural Science Foundation(No.19D3859)the Shanghai Pujiang Talent Program(No.20PJ1400600)the International Joint Laboratory for Advanced Fiber and Low-Dimension Materials(No.18520750400).
文摘Developing efficient,stable and sustainable photocatalysts for water splitting is one of the most significant methods for generating hydrogen.Conjugated microporous polymers,as a new type of organic semiconductor photocatalyst,have adjustable bandgaps and high specific surface areas,and can be synthesized using diverse methods.In this work,we report the design and synthesis of a series of pyridyl conjugated microporous polymers(PCMPs)utilizing polycondensation of aromatic aldehydes and aromatic ketones in the presence of ammonium acetate.PCMPs with different chemical structures were synthesized via adjusting monomers with different geometries and contents of nitrogen element,which could adjust the bandgap and photocatalytic performance.Photocatalytic hydrogen evolution rate(HER)up to 1198.9μmol·h^(-1)·g^(-1) was achieved on the optimized polymer with a specific surface area of 312 m^(2)·g^(-1) under UV-Vis light irradiation(A>320 nm).This metal-free synthetic method provides a new avenue to preparing an efficient photocatalyst for hydrogen evolution.
基金supported by the National Natural Science Foundation of China (52373172, 52073046, and 52103106)the National Key Research and Development Program of China (2022YFB3807100 and 2022YFB3807102)+3 种基金the Program of Shanghai Academic Research Leader (21XD1420200)the Chang Jiang Scholar Program (Liao Y, T2023082)the Natural Science Foundation of Shanghai (23ZR1401100)the State Key Laboratory for Modification of Chemical Fibers and Polymer Materials (KF2204, KF2306, and KF2316)。
文摘The development of trimethylamine (TMA) gassensors is crucial for environmental monitoring, food safety,and health surveillance. However, it is difficult to achievestable detection of TMA with low concentration at a lowtemperature. In this work, a series of conjugated microporouspolytriphenylamine (PTPA) were designed and synthesized,with tunable porosity and surface area, using Hansen solubilityparameters and nanosilica spheres as templates. Comparedto pure PTPA (R = 4 for 100 ppm), the modified PTPAderivatives exhibited significantly enhanced TMA sensingperformance, with NaF-PTPA achieving a remarkable sensitivity(R = 22 for 100 ppm) and a low detection limit of0.53 ppm. The NaF-PTPA based sensor also demonstratedexcellent long-term stability, maintaining consistent performanceover 30 days at 54 °C. The impressive results can beattributed to the protonation (–NH_(2)^(+)), modified porosity andincreased surface area. Hence, this strategy presents new insightsfor the advancement of low-temperature sensing technologies.
