There is, I think, something ethereal about i —the square root of minus one. I remember first hearing about it at school. It seemed an odd beast at that time—an intruder hovering on the edge of reality.

Usually familiarity dulls this sense of the bizarre, but in the case of i it was the reverse: over the years the sense of its surreal nature intensified. It seemed that it was impossible to write mathematics that described the real world in …

I and i

As a fascinating conjugated polymer, graphitic carbon nitride (g-C3N4) has become a new research hotspot and drawn broad interdisciplinary attention as a metal-free and visible-light-responsive photocatalyst in the arena of solar energy conversion and environmental remediation. This is due to its appealing electronic band structure, high physicochemical stability, and “earth-abundant” nature. This critical review summarizes a panorama of the latest progress related to the design and construction of pristine g-C3N4 and g-C3N4-based nanocomposites, including (1) nanoarchitecture design of bare g-C3N4, such as hard and soft templating approaches, supramolecular preorganization assembly, exfoliation, and template-free synthesis routes, (2) functionalization of g-C3N4 at an atomic level (elemental doping) and molecular level (copolymerization), and (3) modification of g-C3N4 with well-matched energy levels of another semiconductor or a metal as a cocatalyst to form heterojunction nanostructures. The constructi...

Graphitic Carbon Nitride (g-C3N4)-Based Photocatalysts for Artificial Photosynthesis and Environmental Remediation: Are We a Step Closer To Achieving Sustainability?

Magneto-optical Kerr effect microscopy is used to show that monolayer chromium triiodide is an Ising ferromagnet with out-of-plane spin orientation. The question of what happens to the properties of a material when it is thinned down to atomic-scale thickness has for a long time been a largely hypothetical one. In the past decade, new experimental methods have made it possible to isolate and measure a range of two-dimensional structures, enabling many theoretical predictions to be tested. But it has been a particular challenge to observe intrinsic magnetic effects, which could shed light on the longstanding fundamental question of whether intrinsic long-range magnetic order can robustly exist in two dimensions. In this issue of Nature, two groups address this challenge and report ferromagnetism in atomically thin crystals. Xiang Zhang and colleagues measured atomic layers of Cr2Ge2Te6 and observed ferromagnetic ordering with a transition temperature that, unusually, can be controlled using small magnetic fields. Xiaodong Xu and colleagues measured atomic layers of CrI3 and observed ferromagnetic ordering that, remarkably, was suppressed in double layers of CrI3, but restored in triple layers. The two studies demonstrate a platform with which to test fundamental properties of purely two-dimensional magnets. Since the discovery of graphene1, the family of two-dimensional materials has grown, displaying a broad range of electronic properties. Recent additions include semiconductors with spin–valley coupling2, Ising superconductors3,4,5 that can be tuned into a quantum metal6, possible Mott insulators with tunable charge-density waves7, and topological semimetals with edge transport8,9. However, no two-dimensional crystal with intrinsic magnetism has yet been discovered10,11,12,13,14; such a crystal would be useful in many technologies from sensing to data storage15. Theoretically, magnetic order is prohibited in the two-dimensional isotropic Heisenberg model at finite temperatures by the Mermin–Wagner theorem16. Magnetic anisotropy removes this restriction, however, and enables, for instance, the occurrence of two-dimensional Ising ferromagnetism. Here we use magneto-optical Kerr effect microscopy to demonstrate that monolayer chromium triiodide (CrI3) is an Ising ferromagnet with out-of-plane spin orientation. Its Curie temperature of 45 kelvin is only slightly lower than that of the bulk crystal, 61 kelvin, which is consistent with a weak interlayer coupling. Moreover, our studies suggest a layer-dependent magnetic phase, highlighting thickness-dependent physical properties typical of van der Waals crystals17,18,19. Remarkably, bilayer CrI3 displays suppressed magnetization with a metamagnetic effect20, whereas in trilayer CrI3 the interlayer ferromagnetism observed in the bulk crystal is restored. This work creates opportunities for studying magnetism by harnessing the unusual features of atomically thin materials, such as electrical control for realizing magnetoelectronics12, and van der Waals engineering to produce interface phenomena15.

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Layer-dependent ferromagnetism in a van der Waals crystal down to the monolayer limit

Since the discovery of mechanically exfoliated graphene in 2004, research on ultrathin two-dimensional (2D) nanomaterials has grown exponentially in the fields of condensed matter physics, material science, chemistry, and nanotechnology. Highlighting their compelling physical, chemical, electronic, and optical properties, as well as their various potential applications, in this Review, we summarize the state-of-art progress on the ultrathin 2D nanomaterials with a particular emphasis on their recent advances. First, we introduce the unique advances on ultrathin 2D nanomaterials, followed by the description of their composition and crystal structures. The assortments of their synthetic methods are then summarized, including insights on their advantages and limitations, alongside some recommendations on suitable characterization techniques. We also discuss in detail the utilization of these ultrathin 2D nanomaterials for wide ranges of potential applications among the electronics/optoelectronics, electrocat...

Recent Advances in Ultrathin Two-Dimensional Nanomaterials

A review on g-C3N4-based photocatalysts

The double perovskite family, A2MIMIIIX6, represents a promising route to overcome the lead toxicity issue confronting current photovoltaic (PV) standout, CH3NH3PbI3 Given the generally large indirect bandgap within most known double perovskites, bandgap engineering provides an important approach for targeting outstanding PV performance within this family Using Cs2AgBiBr6 as host, we demonstrate bandgap engineering through alloying of InIII/SbIII Cs2Ag(Bi1-xMx)Br6 (M = In, Sb) accommodates up to 75% InIII with increased bandgap, and up to 375% SbIII with reduced bandgap—ie, enabling ~041 eV bandgap modulation through introduction of the two metals, with smallest value of 186 eV for Cs2Ag(Bi0625Sb0375)Br6 Band structure calculations indicate that opposite bandgap shift directions associated with Sb/In substitution arise from different atomic configurations for these atoms Associated photoluminescence and environmental stability of the three-metal systems are also assessed

Bandgap Engineering of Lead-Free Double Perovskite Cs 2 AgBiBr 6 through Trivalent Metal Alloying

2D semiconducting metal phosphorus trichalcogenides, particularly the bulk crystals of MPS3 (M = Fe, Mn, Ni, Cd and Zn) sulfides and MPSe3 (M = Fe and Mn) selenides, have been synthesized, crystallized and exfoliated into monolayers. The Raman spectra of monolayer FePS3 and 3-layer FePSe3 show the strong intralayer vibrations and structural stability of the atomically thin layers under ambient condition. The band gaps can be adjusted by element choices in the range of 1.3–3.5 eV. The wide-range band gaps suggest their optoelectronic applications in a broad wavelength range. The calculated cleavage energies of MPS3 are smaller than that of graphite. Therefore, the monolayers used for building of heterostructures by van der Waals stacking could be considered as the candidates for artificial 2D materials with unusual ferroelectric and magnetic properties.

Weak Van der Waals Stacking, Wide-Range Band Gap, and Raman Study on Ultrathin Layers of Metal Phosphorus Trichalcogenides.

A series of two-dimensional (2D) hybrid organic–inorganic perovskite (HOIP) crystals, based on acene alkylamine cations (i.e., phenylmethylammonium (PMA), 2-phenylethylammonium (PEA), 1-(2-naphthyl)methanammonium (NMA), and 2-(2-naphthyl)ethanammonium (NEA)) and lead(II) halide (i.e., PbX42–, X = Cl, Br, and I) frameworks, and their corresponding thin films were fabricated and examined for structure–property relationship. Several new or redetermined crystal structures are reported, including those for (NEA)2PbI4, (NEA)2PbBr4, (NMA)2PbBr4, (PMA)2PbBr4, and (PEA)2PbI4. Non-centrosymmetric structures from among these 2D HOIPs were confirmed by piezoresponse force microscopy—especially noteworthy is the structure of (PMA)2PbBr4, which was previously reported as centrosymmetric. Examination of the impact of organic cation and inorganic layer choice on the exciton absorption/emission properties, among the set of compounds considered, reveals that perovskite layer distortion (i.e., Pb–I–Pb bond angle between adj...

Two-Dimensional Lead(II) Halide-Based Hybrid Perovskites Templated by Acene Alkylamines: Crystal Structures, Optical Properties, and Piezoelectricity.

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Raman spectroscopy of atomically thin two-dimensional magnetic iron phosphorus trisulfide (FePS3) crystals

Uranium is important in the nuclear fuel cycle both as an energy source and as radioactive waste. It is of vital importance to recover uranium from nuclear waste solutions for further treatment and disposal. Herein we present the first chalcogenide example, (Me2NH2)1.33(Me3NH)0.67Sn3S7·1.25H2O (FJSM-SnS), in which organic amine cations can be used for selective UO22+ ion-exchange. The UO22+-exchange kinetics perfectly conforms to pseudo-second-order reaction, which is observed for the first time in a chalcogenide ion-exchanger. This reveals the chemical adsorption process and its ion-exchange mechanism. FJSM-SnS has excellent pH stability in both strongly acidic and basic environments (pH = 2.1–11), with a maximum uranium-exchange capacity of 338.43 mg/g. It can efficiently capture UO22+ ions in the presence of high concentrations of Na+, Ca2+, or HCO3– (the highest distribution coefficient Kd value reached 4.28 × 104 mL/g). The material is also very effective in removing of trace levels of U in the prese...

Ke-Zhao Du

Papers

Bandgap Engineering of Lead-Free Double Perovskite Cs 2 AgBiBr 6 through Trivalent Metal Alloying

Weak Van der Waals Stacking, Wide-Range Band Gap, and Raman Study on Ultrathin Layers of Metal Phosphorus Trichalcogenides.

Two-Dimensional Lead(II) Halide-Based Hybrid Perovskites Templated by Acene Alkylamines: Crystal Structures, Optical Properties, and Piezoelectricity.

Raman spectroscopy of atomically thin two-dimensional magnetic iron phosphorus trisulfide (FePS3) crystals

Efficient Removal and Recovery of Uranium by a Layered Organic-Inorganic Hybrid Thiostannate