Alessandro
Fortunelli
*ab and
Stefan
Vajda
*cdef
aCNR-ICCOM, Consiglio Nazionale delle Ricerche, Pisa, Italy
bMaterials and Process Simulation Center, California Institute of Technology, Pasadena, California, USA. E-mail: alessandro.fortunelli@cnr.it
cMaterials Science Division, Argonne National Laboratory, Argonne, Illinois, USA. E-mail: vajda@anl.gov
dNanoscience and Technology Division, Argonne National Laboratory, Argonne, Illinois, USA
eInstitute for Molecular Engineering, The University of Chicago, Chicago, Illinois, USA
fDepartment of Chemical & Environmental Engineering, School of Engineering & Applied Science, Yale University, New Haven, USA
To face these challenges, recent developments and advances have been realized in three major areas: (i) catalyst preparation and treatment (e.g. size selection and control, high precision synthesis of poly-metallic particles, novel nanostructured systems); (ii) nanostructure characterization (especially in situ/operando characterization of structural, morphological, compositional, and textural properties of catalysts under reaction conditions); and (iii) predictive computational modeling of realistic catalytic systems (in silico screening under operating conditions). To these advances, a fourth should be added, that is, (iv) the synergic and cross-disciplinary combination of the previous three areas to achieve interactions and stronger links among different experimental and theoretical techniques for characterizing, synthesizing, and sampling the chemical behavior of such materials. Indeed, a close coupling of experimental synthetic and characterization methods with theory can form a highly complementary multidisciplinary approach towards the design of new catalytic multifunctional materials. To give a few examples: (i) novel nanostructured systems are continuously being synthesized, such as novel particle/substrate combinations, small sub-nanometer clusters that consist of only a handful of atoms with atomic precision, size- and shape-defined few-nanometer particles, nanoalloy synthesis with controlled composition and ordering, and extensive use of novel preparation and impregnation techniques such as atomic layer deposition or deposition of colloidal systems on supports; (ii) impressive progress has been made with in situ characterization through synchrotron-based X-ray techniques such as absorption fine structure spectroscopy (XAFS), emission (XES) and photoelectron (XPS) spectroscopy, advanced microscopy such as scanning and transmission electron microscopy (SEM and TEM), and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS); and (iii) multi-scale modeling approaches have been and are being developed that, starting from a systematic sampling of reaction paths at the atomistic level, taking explicitly into account realistic reaction conditions of temperature and chemical potentials of reactants, reach the description of processes occurring on macroscopic length scales such as mass and heat transport. The basic idea underlying these developments is that a fundamental understanding of structure/property relationships and of reaction mechanisms at work under realistic conditions can be extremely useful if not tout court indispensable for making progress also in technological applications, to realize an informed rational design which can eventually solve the above-mentioned societal challenges.
These advances have indeed opened novel perspectives in the field for all types of heterogeneous catalysts synthesized under wet chemistry, physical deposition, vacuum or ambient conditions, and have enabled a much deeper understanding of fundamental phenomena such as the evolution of catalytic properties with size and composition, from the smallest atomic clusters consisting only of under-coordinated surface atoms, to middle-sized and larger particles with a changing ratio of facets to corners, edges and core atoms and the associated non-monotonic evolution of propensities to binding, reactivity and catalytic properties, and the associated complex, evolving under reaction conditions, and catalyst structures. Growing evidence is in fact accumulating showing that the status of the catalysts under reaction conditions plays a crucial role in the catalytic activity, hence the need to obtain precise information on how the as-prepared materials evolve once exposed to the reaction environment in terms of the in situ oxidation state, coverage, and structural dynamics.
The present themed issue of Catalysis Science & Technology offers a representative (although by necessity incomplete) selection of contributions which take advantage of these recent developments, and in several cases combine them in a multi-disciplinary effort or discuss them in a broader context and perspective. We thus believe that this issue provides a picture of the state-of-the-art in the field of nanocatalysis, with a balanced mix of applied, fundamental, experimental and computational research, and we hope that it will be of significant interest to both academic and industrial researchers and will trigger further progress in the field, as per our goal in proposing it. For convenience of the reader, Table 1 lists the articles that appear in the printed version of this themed issue, grouped by topic.
Theme | Paper | Topic of the paper | DOI | Approach |
---|---|---|---|---|
(1) Catalysts synthesized by physical methods | ||||
Size-dependent structure | S. Peredkov et al. | Investigation of the structure of metallic and oxidized Cu35 and Cu55 clusters, X-ray absorption spectroscopy | 10.1039/c6cy00436a | Experiment |
Structure and dynamics | Z. Duan et al. | Structure and dynamics of Au147 nanoclusters, X-ray absorption spectroscopy, density functional theory | 10.1039/c6cy00559d | Experiment & theory |
Heterogeneous catalysis | H. Yasumatsu et al. | CO oxidation on Si-supported Pt30 clusters | 10.1039/c6cy00623j | Experiment |
Heterogeneous catalysis | J. Nordheim Riedel et al. | H2/D2 exchange on SiO2-supported Pt8 clusters, effect of O2 | 10.1039/c6cy00756b | Experiment & theory |
Electrocatalysis | R. Passalacqua et al. | Interaction of Cu5 and Cu20 clusters with CO2, voltammetry | 10.1039/c6cy00942e | Experiment |
(2) Materials synthesized via chemical routes | ||||
Catalyst design & synthesis | Z. Lu et al. | Using atomic layer deposition for the design of Pd-based nanocatalysts | 10.1039/c6cy00682e | Experiment |
Properties of thin oxide films | B.-H. Mao et al. | Electronic structure of thin oxide films prepared by atomic layer deposition, interactions with oxygen | 10.1039/c6cy00575f | Experiment |
Heterogeneous catalysis | S.-B. Ivan et al. | Nickel oxide in the oxidative dehydrogenation of ethane, effect of phosphorus on catalyst performance | 10.1039/c6cy00946h | Experiment |
Heterogeneous catalysis | V. Fung et al. | Oxidative dehydrogenation of ethane on Co3O4 nanorods | 10.1039/c6cy00749j | Experiment & theory |
Heterogeneous catalysis | M. Zacharska et al. | Hydrogen production from formic acid on oxide-supported Au nanoclusters | 10.1039/c6cy00552g | Experiment |
Heterogeneous catalysis | X. Yang et al. | Crotonaldehyde hydrogenation on Pt-titania and Pt-ceria nanoparticles | 10.1039/c6cy00858e | Experiment |
Heterogeneous catalysis | M. Keppeler et al. | Reactivity of CO, NO, O2 and C2H6 on zeolite-supported Pt13±2 clusters | 10.1039/c6cy00182c | Experiment |
Heterogeneous catalysis | S. Posada-Pérez et al. | CO2 conversion to methanol on β-Mo2C and Cu/β-Mo2C | 10.1039/c5cy02143j | Experiment & theory |
Heterogeneous catalysis | S. Derrouiche et al. | Selective butadiene hydrogenation on AuZn nanoalloy formed from Au/ZnO | 10.1039/c5cy01664a | Experiment |
Heterogeneous catalysis | Z. Wu et al. | Pd–In inter-metallic alloy nanoparticles: highly selective ethane dehydrogenation catalysts | 10.1039/c6cy00491a | Experiment |
Heterogeneous catalysis | X. Wang et al. | Selective gas phase hydrogenation of nitroarenes over Mo2C-supported Au–Pd | 10.1039/c6cy00514d | Experiment |
Electrocatalysis | H. A. Miller et al. | Hydrogen production by alcohol electroreforming on Au–Pd core shell nanoparticles | 10.1039/c6cy00720a | Experiment |
Photocatalysis | J. C. Matsubu et. al. | Oxygen evolution from water: the effect of the interface on the reactivity of semiconductor-cocatalyst junctions | 10.1039/c6cy00548a | Experiment |
(3) Computational and theoretical studies | ||||
Catalyst stability | A. Figueroba et al. | Stability of ceria-supported single atom Pt, Fe, Ru, Os, Co, Rh, Ir, Ni, Pd, Cu, Ag, and Au catalysts | 10.1039/c6cy00294c | Theory |
Heterogeneous catalysis | J. Nevalaita et al. | Oxygen dissociation on Mo-doped CaO(001) surface and in the presence of Au atoms and clusters | 10.1039/c5cy01839k | Theory |
Heterogeneous catalysis | I. Demiroglu et al. | Absorption of H2, O2 and CO on Au–Rh nanoalloys, size and composition effect, density functional theory | 10.1039/c6cy01107a | Theory |
Heterogeneous catalysis | J.-X. Liang | CO oxidation on single-atom Ni catalyst supported on iron oxide | 10.1039/c6cy00672h | Theory |
Electrochemistry | L. Sementa et al. | Oxygen reduction reaction on Pt38 clusters, molecular dynamics simulations | 10.1039/c6cy00750c | Theory |
We would like to thank all the authors who have contributed to this themed issue, and the editorial team of Catalysis Science & Technology for their kind and punctual assistance. AF acknowledges support by the European Community for the ERC-AdG SEPON project. SV acknowledges support by the U.S. Department of Energy, BES-Materials Sciences, under Contract DE-AC-02-06CH11357, with UChicago Argonne, LLC, the operator of Argonne National Laboratory.
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