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Aromatic alcohols oxidation and hydrogen evolution over π-electron conjugated porous carbon nitride rods

Nano Research 2022年第12期15卷 10148-10157页

作者： Jiawei Xia Neeta Karjule Gabriel Mark Michael Volokh Haiqun Chen Menny Shalom Key Laboratory of Advanced Catalytic Materials and Technology Advanced Catalysis and Green Manufacturing Collaborative Innovation CenterChangzhou UniversityChangzhou213164China Department of Chemistry and Ilse Katz Institute for Nanoscale Science and Technology Ben-Gurion University of the NegevBeer-Sheva8410501Israel

Photocatalysis using polymeric carbon nitride(CN)materials is a constantly evolving field,where the variation of synthetic procedures allows the constant improvement of activity by tackling the intrinsic limitations of these materials(optical absorbance,specific surface area,charge migration,etc.).Amongst the possible photocatalytic reactions,the most popular application of CNs is the hydrogen evolution reaction(HER)from *** this work,we design precisely-controlled carbon-doped porous CN rods with extended π-electron conjugation from supramolecular assemblies of melem and co-monomers,which partially substitute nitrogen for carbon atoms at the pyrimidine ring of the *** hydrogen bonds and good thermal stability of the melem-based supramolecular framework allow synthesizing a more ordered structure for improved charge migration;the control from the molecular level over the position of carbon-substituted nitrogen positions tailors the band alignment and photogenerated charge *** optimal photocatalyst shows an excellent HER rate(up to 10.16 mmol·h-1·g-1 under 100 W white light-emitting diode(LED)irradiation,with an apparent quantum efficiency of 20.0%at 405 nm,which is 23.2 times higher compared to a reference bulk CN).To fully harness the benefits of the developed metal-free CNs,selective oxidation reaction of aromatic alcohols is demonstrated with high conversion and selectivity.

关键词： supramolecular assembly π-electron conjugation carbon nitride photocatalytic hydrogen evolution reaction selective aromatic alcohol oxidation

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General approach for atomically dispersed precious metal catalysts toward hydrogen reaction

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Carbon Energy 2023年第7期5卷 100-111页

作者： Ruisong Li Daoxiong Wu Peng Rao Peilin Deng Jing Li Junming Luo Wei Huang Qi Chen Zhenye Kang Yijun Shen Xinlong Tian State Key Laboratory of Marine Resource Utilization in South China Sea Hainan Provincial Key Lab of Fine ChemistrySchool of Chemical Engineering and TechnologyHainan UniversityHaikouChina

As a carbon-free energy carrier,hydrogen has become the pivot for future clean energy,while efficient hydrogen production and combustion still require precious metal-based ***-atom catalysts(SACs)with high atomic utilization open up a desirable perspective for the scale applications of precious metals,but the general and facile preparation of various precious metal-based SACs remains ***,a general movable printing method has been developed to synthesize various precious metal-based SACs,such as Pd,Pt,Rh,Ir,and Ru,and the features of highly dispersed single atoms with nitrogen coordination have been identified by comprehensive *** importantly,the synthesized Pt-and Ru-based SACs exhibit much higher activities than their corresponding nanoparticle counterparts for hydrogen oxidation reaction and hydrogen evolution reaction(HER).In addition,the Pd-based SAC delivers an excellent activity for photocatalytic hydrogen *** for the superior mass activity of Ru-based SACs toward HER,density functional theory calculations confirmed that the adsorption of the hydrogen atom has a significant effect on the spin state and electronic structure of the catalysts.

关键词： hydrogen evolution reaction hydrogen oxidation reaction photocatalytic hydrogen evolution reaction precious metals single-atom catalysts

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The incorporation of cocatalyst cobalt sulfide into graphitic carbon nitride:Boosted photocatalytic hydrogen evolution performance and mechanism exploration

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Nano Materials Science 2023年第2期5卷 202-209页

作者： Zhangqian Liang Yanjun Xue Xinyu Wang Xiaoli Zhang Jian Tian Hongzhi Cui School of Materials Science and Engineering Shandong University of Science and TechnologyQingdao266590China School of Materials Science and Engineering Zhengzhou UniversityZhengzhou450001China

2D-layered graphitic carbon nitride(g-C_(3)N_(4))is regarded as a great prospect as a photocatalyst for H_(2)***,g-C_(3)N_(4)’s photocatalytic hydrogen evolution(HER)activity is significantly restricted by the recombination of *** find that cobalt sulfide(CoS_(2))as a cocatalyst can promote g-C_(3)N_(4)nanosheets(NSs)to realize very efficient photocatalytic H_(2)*** prepared CoS_(2)/g-C_(3)N_(4)hybrids display highly boosted photocatalytic H_(2)generation performance and outstanding cycle *** optimized 7%-CoS_(2)/g-C_(3)N_(4)hybrids show a much improved photocatalytic H_(2)generation rate of 36.2μmol-1h-1,which is about 180 times as much as bare g-C_(3)N_(4)(0.2μmol-1h-1).In addition,the apparent quantum efficiency(AQE)of all the samples was computed under light atλ=370 nm,in which the AQE of 7%-CoS_(2)/g-C_(3)N_(4)hybrids is up to 5.72%.The experimental data and the DFT calculation suggest that the CoS_(2)/g-C_(3)N_(4)hybrid’s excellent HER activity is attributable to the lower overpotential and the smaller Co-H bond activation energy for ***,the CoS_(2)cocatalyst loading effectively boosts the photocatalytic performance of g-C_(3)N_(4)for H_(2)*** project promotes fast development of high-efficiency photocatalysts and low-cost for photocatalytic H_(2)generation.

关键词： Non-precious-metal cocatalysts photocatalytic hydrogen evolution reaction CoS_(2)cocatalysts 2D-layered g-C_(3)N_(4)

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