Carbon dioxide transformation to fuels or chemicals provides an attractive approach for its utilization as feedstock and its emission reduction. Herein, we report a gas-phase electrocatalytic reduction of CO2 in an electrolytic cell, constructed using phosphoric acid-doped polybenz- imidazole （PBI） membrane, which allowed operation at 170 ℃ Pt/C and PtMo/C with variable ratio of Pt/Mo were studied as the cathode catalysts. The results showed that PtMo/C catalysts significantly enhanced CO formation and inhibited CH4 formation compared with Pt/C catalyst. Characterization by X-ray diffraction, X-ray photoelectron spectroscopy and transmission electron microscopy revealed that most Mo species existed as MoO3 in PtMo/C catalysts and the interaction between Pt and MoOx was likely responsible for the enhanced CO formation rate although these bicomponent catalysts in general had a larger particle size than Pt/C catalyst.
Dunfeng GaoFan CaiQinqin XuGuoxiong WangXiulian PanXinhe Bao
A versatile wet chemistry method is developed for filling of subnanometer sized metal particles in carbon nanotubes with a diameter smaller than 1.5 nm. As an example, we showed that a confined bi-component Pd-V catalyst exhibit a higher benzene hydroxylation activity compared with that within multi-walled carbon nanotubes.
The interface between a two-dimensional(2D)atomic crystal and a metal surface can be regarded as a nanoreactor, in which molecule adsorption and catalytic reactions may occur. In this work, we demonstrate that oxygen intercalation and desorption occur at the interface between hexagonal boron nitride(h-BN) overlayer and Pt(111) surface by using near-ambient pressure X-ray photoelectron spectroscopy(NAP-XPS), photoemission electron microscopy, and low-energy electron microscopy.Furthermore, CO oxidation under the h-BN cover was also observed by NAP-XPS. The present results indicate that the nanospace under the 2D cover can be used for surface reactions, in which novel surface chemistry may be induced by the nanoconfinement effect.
Commercial production of vinyl chloride from acetylene relies on the use of HgCla as the catalyst, which has caused severe environmental problem and threats to human health because of its toxicity. Therefore, it is vital to explore alternative catalysts without mercury. We report here that N-doped carbon can catalyze directly transformation of acetylene to vinyl chloride. Particularly, N-doped high surface area mesoporous carbon exhibits a rather high activity with the acetylene conversion reaching 77% and vinyl chloride selectivity above 98% at a space velocity of 1.0 mL.min-l.g-1 and 200 ~C. It delivers a stable performa℃nce within a test period of 100h and no obvious deactivation is observed, demonstrating potentials to substitute the notoriously toxic mercuric chloride catalyst.
In heterogeneous catalysis, the modulation of catalysis occurring on metal catalysts can be done by changing the electronic structure of the active surface through a modification of its composition and structure of the surface or the sub-surface [1]. Surface alloying is an effective method, and the electronic structure of the metal surface can be tuned by introducing
