Formic acid （HCOOH） decomposition at Pt film electrode has been studied by electrochem- ical in situ FTIR spectroscopy under attenuated-total-reflection configuration, in order to clarify whether bridge-bonded forma...Formic acid （HCOOH） decomposition at Pt film electrode has been studied by electrochem- ical in situ FTIR spectroscopy under attenuated-total-reflection configuration, in order to clarify whether bridge-bonded formate （HCOOD） is the reactive intermediate for COad for-mation from HCOOH molecules. When switching from HCOOH-free solution to HCOOH- containing solution at constant potential （E=0.4 V vs. RHE）, we found that immediately upon solution switch COad formation rate is the highest, while surface coverage of formate is zero, then after COad formation rate decreases, while formate coverage reaches a steady state coverage quickly within ca. 1 s. Potential step experiment from E=0.75 V to 0.35 V, reveals that formate band intensity drops immediately right after the potential step, while the COad signal develops slowly with time. Both facts indicate that formate is not the reactive intermediate for formic acid dehydration to CO.展开更多
The configuration of[PdCl_2(C_2H_4OH)]^- has been studied by pseudopotential ab initio method.A cis isomer was found to be the reaction intermediate in the Wacker process.
To validate the ability of full configuration interaction quantum Monte Carlo （FCIQMC） for studying the 2D Hubbard model near half-filling regime, the ground state energies of a 4×44×4 square lattice syste...To validate the ability of full configuration interaction quantum Monte Carlo （FCIQMC） for studying the 2D Hubbard model near half-filling regime, the ground state energies of a 4×44×4 square lattice system with various interaction strengths are calculated. It is found that the calculated results are in good agreement with those obtained by exact diagonalization （i.e., the exact values for a given basis set） when the population of psi particles （psips） is higher than the critical population required to correctly sample the ground state wave function. In addition, the variations of the average computational time per 20 Monte Carlo cycles with the coupling strength and the number of processors are also analyzed. The calculated results show that the computational efficiency of an FCIQMC calculation is mainly affected by the total population of psips and the communication between processors. These results can provide useful references for understanding the FCIQMC algorithm, studying the ground state properties of the 2D Hubbard model for the larger system size by the FCIQMC method and using a computational budget as effectively as possible.展开更多
文摘Formic acid （HCOOH） decomposition at Pt film electrode has been studied by electrochem- ical in situ FTIR spectroscopy under attenuated-total-reflection configuration, in order to clarify whether bridge-bonded formate （HCOOD） is the reactive intermediate for COad for-mation from HCOOH molecules. When switching from HCOOH-free solution to HCOOH- containing solution at constant potential （E=0.4 V vs. RHE）, we found that immediately upon solution switch COad formation rate is the highest, while surface coverage of formate is zero, then after COad formation rate decreases, while formate coverage reaches a steady state coverage quickly within ca. 1 s. Potential step experiment from E=0.75 V to 0.35 V, reveals that formate band intensity drops immediately right after the potential step, while the COad signal develops slowly with time. Both facts indicate that formate is not the reactive intermediate for formic acid dehydration to CO.
文摘The configuration of[PdCl_2(C_2H_4OH)]^- has been studied by pseudopotential ab initio method.A cis isomer was found to be the reaction intermediate in the Wacker process.
基金Supported by the Natural Science Foundation for Colleges and Universities of Jiangsu Province under Grant No 16KJB140008the National Natural Science Foundation of China under Grant Nos 11447204 and 11647164+1 种基金the Natural Science Foundation of Jiangsu Province under Grant No BK20151079the Scientific Research Foundation of Nanjing Xiaozhuang University under Grant No 2015NXY34
文摘To validate the ability of full configuration interaction quantum Monte Carlo （FCIQMC） for studying the 2D Hubbard model near half-filling regime, the ground state energies of a 4×44×4 square lattice system with various interaction strengths are calculated. It is found that the calculated results are in good agreement with those obtained by exact diagonalization （i.e., the exact values for a given basis set） when the population of psi particles （psips） is higher than the critical population required to correctly sample the ground state wave function. In addition, the variations of the average computational time per 20 Monte Carlo cycles with the coupling strength and the number of processors are also analyzed. The calculated results show that the computational efficiency of an FCIQMC calculation is mainly affected by the total population of psips and the communication between processors. These results can provide useful references for understanding the FCIQMC algorithm, studying the ground state properties of the 2D Hubbard model for the larger system size by the FCIQMC method and using a computational budget as effectively as possible.
