Conspectus
C1 catalysis, which refers to
the conversion of molecules with a single carbon atom, such as CO,
CO2, and CH4, into clean fuels and basic building
blocks for chemical industries, has built a bridge between carbon
resource utilization and valuable chemical supply. With respect to
the goal of carbon neutrality, C1 catalysis also plays an essential
role owing to its integrated functions in the green catalytic process
with fewer CO2 emissions and even direct high-value-added
utilization of greenhouse gases (CO2 and CH4). However, the inert nature of the C–O or C–H bond
in C1 molecules as well as uncontrollable C–C coupling render
C1 catalysis challenging. The rational design of highly active catalytic
materials (denoted as C1 catalysts) with strong capacities for C–O
or C–H bond activation and C–C coupling by convenient
nanomaterials fabrication methods to boost the catalytic performance
of C1 molecule conversion, including targeted product selectivity
and long-term stability, is the cornerstone of C1 catalysis.
Notably, the familiar concepts in heterogeneous catalysis, such as
tandem catalysis and confinement catalysis, are applicable for C1
catalysis and have been successfully used to design a C1 catalyst.
Regarding the tandem catalysis concept that integrates multiple reactions
in a single-pass via a bi- or multifunctional catalyst, it is promising
to shed new light on the oriented conversion of C1 molecules, especially
for C2+ hydrocarbon or oxygenate synthesis. The confinement
effect is powerful for controlling the product distribution and enhancing
activation efficiency of inert chemical bonds in C1 catalysis due
to the unique reactants/intermediate adsorption and
evolution behaviors on the confined catalytic interface with a special
electronic environment. Moreover, metal–support interactions
(MSIs), electronic properties of the active site, and catalytic engineering
issues are also susceptible to the C1 molecule conversion performance.
Therefore, under the guidance of basic and novel rules in heterogeneous
catalysis, the innovation of catalytic materials with the aid of advanced
catalytic materials fabrication techniques has always been a hot research
topic in C1 catalysis.
In this Account, we briefly describe
the challenges in thermal–catalytic C1 molecule (mainly CO,
CO2, and CH4) conversion. At the same time,
the synergistic functioning of the physicochemical properties of the
catalytic materials on the performance in C1 molecule conversion is
highlighted. More importantly, we summarize our progress in rationally
designing tailor-made C1 catalysts to enhance C1 molecule activation
efficiency and targeted product selectivity via powerful nanomaterials
fabrication techniques, such as traditional wet-chemistry strategies,
the magnetron sputtering method, and 3D printing technology. Specifically,
the ingenious capsule catalyst and ammonia pools in zeolites fabricated
by a wet chemistry process possess an extraordinary effect on the
transformation of CO, CO2, and CH4 molecules.
Also, the sputtering m...