Reducing sizes of precious metals and utilization of the mixed small clusters of them as catalysts in reactions are important methods due to more active sites for higher catalytic eciency.Based on rst-principles calc...Reducing sizes of precious metals and utilization of the mixed small clusters of them as catalysts in reactions are important methods due to more active sites for higher catalytic eciency.Based on rst-principles calculations in this work,we found that the platinumbased clusters of Pt3X(X=Al,Si,Cu)which have the magic number 4 can e ectively catalyze the water decomposition and hydrogen production in just one-step reaction process.The adsorbates of the H2O@Pt3X clusters have strong absorption in the ultraviolet and visible regions with wavelength from 300 nm to 760 nm,indicating the sunlight can be used to drive catalytic hydrolysis for producing clean hydrogen.In addition,the O atom remains on the clusters after hydrolysis and can react with CO to form CO2 in activation barrier of 0.340.58 eV,showing the recycling ability of the products after hydrolysis for eliminating the"poisoning"CO by oxidation.Moreover,the formed CO2 molecule can be detached from the Pt3X clusters at 323 K.Our results provide interesting guidance for practical designing the useful photocatalysts.展开更多
基金supported by the National Natural Science Foundation of China(No.22173052 and No.21933002)the Shandong Provincial Natural Sci-ence Foundation(No.ZR2019BB069).
基金supported by the National Natural Science Foundation of China(Nos.22073042,22122302,U1932147 to Xixi Hu,and No.21733006 to Daiqian Xie)the Fundamental Research Funds for the central universities(No.14380020)。
基金supported by the National Key R&D Program of China(No.2017YFA0303502)the National Natural Science Foundation of China(No.21773221 and No.21727804)the Fundamental Research Funds for the Central Universities of China(No.WK2340000078)。
基金the National Natural Science Foundation of China(No.91536105,No.11174186,and No.11074147)the Tianshan Scholar Program.
文摘Reducing sizes of precious metals and utilization of the mixed small clusters of them as catalysts in reactions are important methods due to more active sites for higher catalytic eciency.Based on rst-principles calculations in this work,we found that the platinumbased clusters of Pt3X(X=Al,Si,Cu)which have the magic number 4 can e ectively catalyze the water decomposition and hydrogen production in just one-step reaction process.The adsorbates of the H2O@Pt3X clusters have strong absorption in the ultraviolet and visible regions with wavelength from 300 nm to 760 nm,indicating the sunlight can be used to drive catalytic hydrolysis for producing clean hydrogen.In addition,the O atom remains on the clusters after hydrolysis and can react with CO to form CO2 in activation barrier of 0.340.58 eV,showing the recycling ability of the products after hydrolysis for eliminating the"poisoning"CO by oxidation.Moreover,the formed CO2 molecule can be detached from the Pt3X clusters at 323 K.Our results provide interesting guidance for practical designing the useful photocatalysts.
基金supported by the National Natural Science Foundation of China(No.21873062)the Fundamental Research Funds for the Central Universities(GK202001009)+2 种基金the Natural Science Basis Research Plan in Shaanxi Province of China(No.2020JM-295)the 111 Project(B14041)Program for Changjiang Scholars and the Innovative Research Team in University(IRT-14R33)。
基金supported by the National Nature Science Foundation of China(No.11674303 and No.11574293)the USTC Center for Micro and Nanoscale Research and Fabrication
基金supported by the National Natural Science Foundation of China (No.21327804, No.21773299, No.91121006, No.21573279, No.11574351, No.11774385, No.11674355, No.21503270, and No.21303255)
基金supported by the National Key R&D Program of China (No.2016YFF0200500)the National Natural Science Foundation of China (No.21473173, No.21590802, No.21403207, No.21503206)the Strategic Priority Research Program of Chinese Academy of Sciences (No.XDB17000000)
基金This work was supported by the National Natural Science Foundation of China （No.21177041 and No.21107026）, the Fundamental Research Funds for the Central Universities （No.2013ZZ0073）, and the Scientific Research Foundation for Returned Overseas Chinese Scholars, State Education Ministry.
基金This work was supported by the Foundation for scholar of Hefei Normal University （No.2014rcjj03）, the Foundations of Educational Committee of Anhui Province （No.KJ2014A205）, the National Natural Science Foundation of China （No.21101053, No.21101054, No.20934004, No.91127046, and No.20874094）, the One Hundred Talent Project of Chinese Academy of Sciences, and the National Basic Research Program of China （No.2012CB821500 and No.2010CB934500）.
基金This work was supported by the National Natural Science Foundation of China （No.21072053 and No.20772028） and the Scientific Research Fund of Hunan Provincial Education Department （No.10K025 and No.09C386）.
基金Acknowledgment： This work was supported by the National Natural Science Foundation of China （No.21076204） and the Basic Research Foundation of Xi＇an University of Architecture and Technology （No.JC1107）.
