Materials have transformed the history of humankind, from the Stone and Bronze Ages to the Silicon Age. While they have continuously taken new forms and levels of integration—from bulk tools to specialized additives to nanoscale devices—materials continue to innovate and drive the progress of human society. At the same time, our understanding of materials—their crystal and electronic structures as well as their (often correlated) properties—has evolved tremendously over the past decades. This is in large part due to the significant progress in the development of characterization tools we have at our disposal, including modern x-ray and neutron scattering techniques that can be applied to both (semi-)crystalline and amorphous materials. The increase in precision analysis of materials is mirrored by an ever-increasing materials scope that has become accessible over the past decades. Thousands, in fact millions, of new materials have been discovered and characterized, and the power of the Periodic Table has been harnessed to access new multinary and hybrid compounds with unparalleled complexity, in terms of both structures and properties. In fact, materials discovery has become a premier discipline on its own right, driven by the vast amounts of tabulated data deposited in global databases, enabled by the vastly enhanced computational power and exquisite refinement of computational tools, in terms of both precision and system size that can be computed.

The kaleidoscope of materials that has defined the progress of materials chemistry over the past 50 years includes transition metal oxides; zeolites; carbon allotropes, such as carbon nanotubes, fullerenes, and graphene; 2D materials beyond graphene, such as transition metal dichalcogenides; porous molecular frameworks, such as metal–organic frameworks (MOFs) and covalent organic frameworks (COFs); and most recently hybrid organic–inorganic perovskites.

There are only few key figures in materials chemistry who have left their fingerprint on essentially all of these materials classes—one of them is Professor Sir Anthony Kevin Cheetham, who has shaped the materials arena for more than 50 years.1 Professor Cheetham’s journey began in the late 1960s at the University of Oxford, and since then, his contributions have defined and directed the evolution of materials chemistry on a global scale. At the forefront of his achievements is his pioneering work on the development and characterization of novel materials. His research has advanced our understanding of crystalline materials and opened new avenues to their characterization by x-ray and neutron diffraction, most prominently reflected by his pioneering work on ab initio structure solution from powder data using neutron and synchrotron x-ray diffraction.2,3 Of no less significance are his landmark contributions to the design and synthesis of new materials with unprecedented properties. Professor Cheetham has discovered numerous metal oxides and studied them for their optical, magnetic, dielectric, and catalytic properties.4,5 His extensive work on the structure and dynamics of nanoporous inorganic solids, including aluminosilicates such as zeolites, and open-framework phosphates, has pushed the rational design of adsorbents and catalysts with tailored properties, a vital prerequisite for the widespread industrial utilization of nanoporous solids.6 Likewise, Professor Cheetham has shaped the field of MOFs,7 a class of materials renowned for their exceptional porosity and diverse applications, and related hybrid materials, including hybrid organic–inorganic perovskites.8 The impact of these hybrid materials extends far beyond the laboratory, holding promise for addressing real-world challenges, such as sustainable energy storage, photovoltaics, and environmental remediation. Professor Cheetham’s seminal work on ferroelectric,9 multiferroic,10 and mechanical properties11 of MOFs has opened up new facets of MOF chemistry, which have quickly been internalized by the MOF community. A recent highlight of his work—the remarkable sorption properties of the earth-abundant MOF aluminum formate, which has been used for CO2 capture from hydrocarbon mixtures, for non-cryogenic air separation to afford oxygen, and for hydrogen storage—has opened up new perspectives for large-scale sorption and separation applications of MOFs in realistic scenarios.12 

With his commitment to advancing the frontiers of science, Professor Cheetham has pioneered and led the field of materials chemistry for decades, leaving a lasting mark on both academia and industry. Likewise, Professor Cheetham’s influence extends globally through his extensive network of collaborations, leadership, mentorship, and advisory roles. As a distinguished professor at leading institutions, such as the University of Cambridge; the University of California at Santa Barbara (UCSB), where he was the Founding Director of the renowned Materials Research Laboratory; and, most recently, the National University of Singapore (NUS), he has nurtured generations of researchers and fostered a culture of collaboration, innovation, and scientific inquiry. His mentorship has inspired a legion of scientists who continue to push the boundaries of science in their own right.

With this Special Issue on the occasion of his 75th Birthday, we celebrate Professor Cheetham’s defining role in materials chemistry across the globe for more than 50 years. This Special Collection embraces materials chemistry in its entire breadth and depth—in terms of materials classes, characterization techniques, and the close entanglement of experiment and theory. In keeping with the unique scope of materials chemistry pioneered by Professor Cheetham, the materials classes reported in this Special Issue span from MOFs to zeolites and metal oxides, borides (Hu et al.13 and Kalyon et al.14), and fluorides, and from DNA mesogens (Gallagher et al.15) to polyaniline (Sonu et al.16) and molecular organic crystals (Mu et al.17).

One prominent theme of this Special Issue revolves around phase (trans)formations, polymorphism, and thermal properties of solids. These include studies on the origin of negative thermal expansion in ScF3 (Dove et al.18), the guest-responsive (negative) thermal expansion behavior of the Zr-porphyrin MOF PCN-222 (Boström et al.19), and the discovery of a new low-temperature tetragonal polymorph of CaZrF6 by Bodine and Wilkinson,20 which, in contrast to the high-temperature cubic form, displays positive thermal expansion in all directions.

Pallach et al.21 report on the complex, entropy-driven phase change behavior of the alkoxy-functionalized MOF, MOF-5, which shows a temperature- and guest-responsive behavior as exemplified by the temperature-induced switching between a “dry,” semi-/non-crystalline aperiodic structure and a highly crystalline cubic structure, driven by increased vibrational and conformational entropy. Kronawitter et al.22 identify the principles guiding the synthesis and glass forming properties of coordination polymers (CPs). They use Li dicyanamide as a eutectic forming glass modifier to tune the thermal properties of the new molecular perovskite [(C3H7)3N(C4H9)]Mn(C2N3)3 (with [C2N3] = dicyanamide, DCA), thus highlighting interesting perspectives for the scalable synthesis of CP glasses and for rationally tuning their macroscopic properties. Staying within the realm of amorphous CPs, correlations between the composition, structure, and mechanical properties of amorphous zeolitic imidazolate frameworks (a-ZIFs) have been computed by Shi et al.23 using a combination of the continuous random network model and large-scale ab initio calculations. The authors deconvolute the distinct effects of short-, medium-, and long-range order on the elastic properties of a-ZIFs, which opens up new perspectives for the rational design of high-strength and high-toughness MOF glasses.

Li et al.24 report the new hybrid-perovskite (R-3AQ)KI3 [R-3AQ2+ = (R)-(+)-3-aminoquinuclidine], which exhibits a reversible order–disorder phase transition and benign mechanical properties suitable for sensing applications. The work by Yuan et al.25 explores the phase space of the hybrid perovskite copper(II) guanidinium formate by density functional theory and shows that a hypothetical polymorph that is isotypic with the most stable polymorph of KCuF3 has a higher free energy than the observed structure. This work pinpoints differences in the structural chemistry of hybrid vs inorganic perovskites and reveals why certain phases that are theoretically plausible cannot be experimentally realized when replacing atomic ions in inorganic perovskites by molecular ions in hybrid perovskites. While revealing the complex phase behavior of inorganic and hybrid solids, these studies also demonstrate the myriad opportunities of rational phase and crystal engineering that can be harnessed to tune the catalytic, magnetic, or optoelectronic properties of inorganic and hybrid solids. For example, Tiyawarakul et al.26 utilize a crystal–glass phase transformation in the 1D CP, ZnPBIm, via melt quenching to macroscopically shape monolithic heterogeneous catalysts for the esterification of levulinic acid.

Another prominent theme of this Special Issue is applying theoretical calculation tools to explore trends in stability, structure–property relationships, and atomistic mechanisms and to discover new materials. Miller and Rondinelli27 asses the global instability index (GII) as a global indicator for structural stability. The authors compute the GII for thousands of compounds in inorganic structure databases and partition compounds by chemical interactions underlying their stability to understand the GII values and their variations. The results of this work show that the GII is suitable for comparisons within controlled datasets but unsuitable as an absolute, universal metric for structural feasibility. Gallagher et al.15 use numerical simulations to explore the phase behavior of different linear DNA constructs. This work provides a useful approach to “design” the phase behavior of DNA constructs by a suitable choice of the constituent nucleotide sequence. DelloStritto et al.28 predict the properties of NiO using density functional theory (DFT) calculations and investigate the impact of various correlation and exchange approximations on its properties. The work by Jiang et al.29 comprehensively assesses the thermodynamic stabilization, local order/disorder, and lattice distortion of a series of compositionally complex Ruddlesden–Popper layered perovskites. Summer et al.30 perform reverse Monte Carlo simulations to analyze the distribution of cations and examine the possibility of oxide-ion disorder of two ceria-zirconia solid solutions based on neutron and x-ray total scattering data. Mu et al.17 adopt a fragment charge difference method to investigate the charge transfer properties of tetrathiafulvalene-based crystals and demonstrate the significant influence of both structure and chemistry on their charge transfer properties, which provides an avenue to quantify charge transfer properties for organic crystals. Zhang et al.31 review the research progress on the discovery of MOFs through high-throughput and machine learning approaches and provide important insights into the future capability of data-driven techniques for MOF discovery. In addition, to address the problem of the MgGa acceptor compensated extensively by the formation of nitrogen vacancies and Mg interstitials in the p-type conductor, GaN:Mg, Xie et al.32 use theoretical calculations to demonstrate that such a compensation can be overcome by forming two kinds of Mg-rich complexes: one that contains nitrogen vacancies and the other that contains only MgGa and Mg interstitials.

Research on the properties and applications of magnetic materials is another important theme of this Special Issue. Examples include studies on the single crystal structure and spin-canted magnetic behavior of α-MnB reported by Kalyon et al.,14 the complex magnetic ordering behavior of the double perovskite Ba2MnMoO6 using a combination of local and crystallographic probes by Coomer et al.,33 and the magnetocaloric effect of the lanthanide fluorides (Dixey et al.34). In addition, Nandwana and Dravid35 demonstrate that the magnetic properties of the ferrite-spinel-based magnetic nanostructures can be enhanced by tuning their crystal chemistry and these nanostructures can act as a contrast agent in magnetic resonance imaging. The work by de h-Óra et al.36 reports cobalt ferrite nanopillars with highly cyclable voltage control of magnetism, which can be used as interconnected synapses for advanced neuromorphic computing applications. Panda et al.37 report a family of Dion–Jacobson hybrid manganese halide perovskites with both long-range magnetic ordering and high photoluminescence quantum yield and investigate the impact of organic amine cations on their photoluminescence and magnetic properties. Li et al.38 prepare multiferroic oxygen storage materials, LnFe3+Mn3+O4.5 (Ln = Y, Lu, and Yb), and explore their structural changes and magnetic properties upon oxidation. These materials exhibit obvious structural modulation that can be attributed to a displacement wave in the fully oxidized compound and exhibit a clear spin glassy behavior.

Other important themes are included in this Special Issue, many showing a clear path toward applications of solid-state materials in such important fields as environmental science or electrochemical energy storage. For example, some invitees showcase materials that are capable of removing Cs+ from nuclear wastewater. Ito et al.39 report the synthesis of the superparamagnetically modified zeolite chabazite using a novel solvothermal route, which shows excellent performance for the removal of Cs+ from radioactively contaminated water. Nearchou et al.40 prepare Sb- and Nb-doped umbites using hydrothermal synthesis and find that these materials display excellent removal of Cs+ cations from acidic, neutral, and basic solutions even in the presence of competing Na+ cations. Some other invitees report the preparation and applications of new electronic or ionic materials. For example, Ramos et al.41 report the new ion conductor Na11Sn2SbSe12, which is a possible candidate as a solid catholyte in composite cathodes for all-solid state Na-batteries. Meanwhile, the authors reveal the complex structure–property relationships governing ion transport in this material. O’Sullivan et al.42 report the structural, optical, and electrical properties of metallic pyrochlore bismuth ruthenate epitaxial heterostructures. Through comprehensive experiments and calculations, these heterostructures are shown to possess semi-metallic properties. Maier43 investigates the cell voltage of mixed conductors under partially frozen conditions, derives the evaluation formulas, and applies these conclusions to hybrid halide perovskites, giving suggestions for refinement of the defect-chemical analysis at very low values of chemical potential. Hu et al.13 explore the hardness and high-pressure behavior of osmium- and ruthenium-doped ReB2 solid solutions and demonstrate that these solid solutions exhibit higher incompressibility and differential strain than pure ReB2, which can be attributed to the reinforced lattice plane after doping. Pramoda and Rao44 review the progress of hetero-superlattices generated by the electrostatic restacking of 2D materials, including MoS2/graphene, MnO2/Ti3C2, Ti3C2/graphene, NiAl–layered double hydroxides/graphene, and NiAl–LDHs/Ti3C2, and their energy applications in supercapacitors, water splitting, and battery cathodes. Vincent et al.45 review MoO3, MoO2, and the series of reduced Mo oxides with intermediate compositions for their performance as Li-ion battery electrode materials. Finally, by analyzing the acoustic emission spectra of kidney stones and porous materials, Eckstein et al.46 conclude that the dynamic failure patterns, which have been identified in earthquakes, magnetism, and switching of ferroelastic and ferroelectric materials, are equally important in medicine and minerals.

In addition, some contributions cover the exploration of advanced preparation processes. Sonu et al.16 present a simple approach to achieve autonomous temporal regulation of polyaniline films’ optical and electrical states by integrating enzyme-catalyzed biochemical reactions. The enzymatic reaction produces a feedback-induced transient pH profile, and correspondingly, the functional states of polyaniline films give rise to a similar switching profile, whose lifetime could be preprogrammed via enzyme concentration. This autonomous, temporally regulated polymer film system represents an advancement to the existing switchable materials that operate at equilibrium. Huang et al.47 use ultrasonic liquid-phase exfoliation and hydrothermal treatments to synthesize fluorescent antimonene quantum dots. The as-prepared dots exhibit good fluorescence characteristics and stability under different salt concentrations. In particular, the quantum dots show high selectivity and rapid detection of Fe3+, CrO42−, and Cr2O72− ions in an aqueous solution with good anti-interference ability. Foo et al.48 achieve the production of monodisperse and pure CsPbBr3 nanocrystals with precise size and shape control under ambient conditions using a mixed passivation strategy. This work offers a cheap and viable approach for the preparation of perovskite nanocrystals in optical and electrical devices. Netzsch et al.49 develop a new strategy for the controllable growth of ZIF-8 nanoparticles on swollen two-dimensional zeolites. This work extends the assembly–disassembly–organization–reassembly concept toward novel hybrid materials, emphasizing the potential that this method provides in synthesizing new materials.

In summary, this Special Issue encompasses modern materials chemistry in all its breadth and depth and, as such, perfectly mirrors Professor Cheetham’s diverse contributions to this important area of science over the past half-century. The guest editors would like to thank Professor Judith Driscoll of the University of Cambridge, UK, who gave us the opportunity to organize this Special Issue, and we are grateful to all authors and editorial staff at APL Materials who gave us their generous support along the way.

Bettina V. Lotsch: Writing – original draft (lead). Jingwei Hou: Writing – review & editing (supporting). Efrain E. Rodriguez: Writing – review & editing (supporting). Wei Li: Writing – original draft (equal).

Data sharing is not applicable to this article as no new data were created or analyzed in this study.

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48.
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