Single-atom catalysis is a hot new area of research. But what is it? According
to an article in Nature Reviews Chemistry titled Heterogeneous
single-atom catalysis …
“Single-atom catalysis,
the catalysis by single-atom catalysts (SACs), has attracted considerable attention
in recent years as a new frontier in the heterogeneous catalysis field. SACs
have the advantages of both homogeneous catalysts (isolated active sites) and
heterogeneous catalysts (stable and easy to separate), and are thus predicted
to be able to bridge the homo- and heterogeneous catalysis.”
TIP #1:
Google® Scholar email alert: Chunshan Song. It was the result of this alert
that I found the article below. And it was this article that made me curious to find out more about single-atom catalysis.
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Preassembly Strategy To Fabricate Porous Hollow Carbonitride
Spheres Inlaid with Single Cu–N3 Sites for Selective Oxidation of Benzene to
Phenol
Ting Zhang†, Di Zhang†,
Xinghua Han‡, Ting Dong‡, Xinwen Guo† , Chunshan Song†? , Rui Si*§, Wei Liu#,
Yuefeng Liu*# , and Zhongkui Zhao*†
† State Key Laboratory of Fine Chemicals, PSU-DUT Joint Center for Energy
Research, School of Chemical Engineering, Dalian University of Technology,
Dalian 116024, P. R. China
‡ School of Chemical Engineering and Technology, North University of China,
Taiyuan 030051, P. R. China
? EMS Energy Institute, PSU-DUT Joint Center for Energy Research and Department
of Energy & Mineral Engineering and Chemical Engineering, Pennsylvania
State University, University Park, Pennsylvania 16802, United States
§ Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied
Physics, Chinese Academy of Sciences, Shanghai 201204, P.R. China
# Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical
Physics, Chinese Academy of Sciences, Dalian 116023, P. R. China
J. Am. Chem. Soc., Article ASAP
Publication Date (Web): November 30, 2018
*sirui@sinap.ac.cn, *yuefeng.liu@dicp.ac.cn, *zkzhao@dlut.edu.cn
Abstract
Developing single-atom catalysts with porous micro-/nanostructures for high
active-site accessibility is of great significance but still remains a
challenge. Herein, we for the first time report a novel template-free
preassembly strategy to fabricate porous hollow graphitic carbonitride spheres
with single Cu atoms mounted via thermal polymerization of supramolecular
preassemblies composed of a melamine–Cu complex and cyanuric acid. Atomically
dispersed Cu–N3 moieties were unambiguously confirmed by spherical aberration
correction electron microscopy and extended X-ray absorption fine structure
spectroscopy. More importantly, this material exhibits outstanding catalytic
performance for selective oxidation of benzene to phenol at room temperature,
especially showing phenol selectivity (90.6 vs 64.2%) and stability much higher
than those of the supported Cu nanoparticles alone, originating from the
isolated unique Cu–N3 sites in the porous hollow structure. An 86% conversion
of benzene, with an unexpectedly high phenol selectivity of 96.7% at 60 °C for
12 h, has been achieved, suggesting a great potential for practical
applications. This work paves a new way to fabricate a variety of single-atom
catalysts with diverse graphitic carbonitride architectures.
source: https://pubs.acs.org/doi/abs/10.1021/jacs.8b10703
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TIP #2:
If you, like me, are new to the concept, Google® What is single-atom catalysis? for more
background. Here is one of the hits from the search …
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Review Article |
Published: 24 May 2018
Heterogeneous
single-atom catalysis
Aiqin Wang, Jun Li & Tao Zhang
Nature Reviews Chemistry volume 2, pages65–81 (2018)
Abstract
Single-atom catalysis has arguably become the most active new frontier in
heterogeneous catalysis. Aided by recent advances in practical synthetic
methodologies, characterization techniques and computational modelling, we now
have a large number of single-atom catalysts (SACs) that exhibit distinctive
performances for a wide variety of chemical reactions. This Perspective
summarizes recent experimental and computational efforts aimed at understanding
the bonding in SACs and how this relates to catalytic performance. The examples
described here illustrate the utility of SACs in a broad scope of industrially
important reactions and highlight the advantages these catalysts have over
those presently used. SACs have well-defined active centres, such that unique
opportunities exist for the rational design of new catalysts with high
activities, selectivities and stabilities. Indeed, given a certain practical
application, we can often design a suitable SAC; thus, the field has developed
very rapidly and afforded promising catalyst leads. Moreover, the control we
have over certain SAC structures paves the way for designing base metal
catalysts with the activities of noble metal catalysts. It appears that we are
entering a new era of heterogeneous catalysis in which we have control over
well-dispersed single-atom active sites whose properties we can readily tune.
source: https://www.nature.com/articles/s41570-018-0010-1
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