Identification of single-site gold catalysis in acetylene hydrochlorination.
نویسندگان
چکیده
There remains considerable debate over the active form of gold under operating conditions of a recently validated gold catalyst for acetylene hydrochlorination. We have performed an in situ x-ray absorption fine structure study of gold/carbon (Au/C) catalysts under acetylene hydrochlorination reaction conditions and show that highly active catalysts comprise single-site cationic Au entities whose activity correlates with the ratio of Au(I):Au(III) present. We demonstrate that these Au/C catalysts are supported analogs of single-site homogeneous Au catalysts and propose a mechanism, supported by computational modeling, based on a redox couple of Au(I)-Au(III) species.
منابع مشابه
Gold - Catalysed Reactions
In recent years, there have been three significant pieces of research which helped propel gold catalysis research into the forefront: the discoveries that gold/silica can catalyse the hydrogenation of pentene, that gold on carbon can be used in the hydrochlorination of acetylene and that deposition-precipitation (DP) methods can be used to prepare nanogold on titania capable of enabling the oxi...
متن کاملTrimetallic Au-Cu-La/AC for Acetylene Hydrochlorination in a Multi-Tubular Fixed Bed Reactor
The metal chloride of LaCl3 was chosen to modify the Au-Cu/AC to decrease the noble metal of gold and enhance the catalytic performances. Then a mercury-free catalyst of Au-Cu-La/AC was prepared by the impregnation method, and the fresh Au-Cu-La/AC and Au-Cu/AC catalysts were also characteri...
متن کاملEnhancement of the Stability of Au-Cu/AC Acetylene Hydrochlorination Bimetallic Catalyst with Melamine Treated Support
This paper highlights the experimental and theoretical studies on the Melamine treated Active Carbon (MAC) support for an Au-Cu bimetallic catalyst in acetylene hydrochlorination reaction. Compared to the original Active Carbon (AC) loaded with the same amount of 0.1wt% Au and 1.0wt% Cu, MAC supported catalyst(MACH), wherein Carbon/C6...
متن کاملModifications of the metal and support during the deactivation and regeneration of Au/C catalysts for the hydrochlorination of acetylene
The effect of gold oxidation state and carbon structure on the activity of Au/C catalyst for the hydrochlorination of acetylene was investigated by a combined approach using TPR, XPS and porosimetry determinations. The activity of the catalyst in the synthesis of vinyl chloride monomer was found to be dependent from the presence of Au 3+ species into the catalyst. However, by preparing catalyst...
متن کاملذخیره در منابع من
با ذخیره ی این منبع در منابع من، دسترسی به آن را برای استفاده های بعدی آسان تر کنید
برای دانلود متن کامل این مقاله و بیش از 32 میلیون مقاله دیگر ابتدا ثبت نام کنید
ثبت ناماگر عضو سایت هستید لطفا وارد حساب کاربری خود شوید
ورودعنوان ژورنال:
- Science
دوره 355 6332 شماره
صفحات -
تاریخ انتشار 2017