Two‐dimensional transition metal carbonitrides (MXene) have demonstrated great potential in many fields. However, the serious aggregation and poor thermodynamic stability of MXene greatly hinder their applications. Here, an interface‐induced self‐assembly strategy to synthesize ordered mesoporous carbon/Ti3C2Tx heterostructures (OMCTs) was developed. In this method, the composite monomicelles formed by Pluronic F127 and low‐molecular‐weight phenolic resol self‐assembled on the surface of Ti3C2Tx to prevent the restacking of Ti3C2Tx and maintain its thermostability. The obtained OMCTs possessed high specific surface areas (259–544 m2 g−1), large pore volumes (0.296–0.481 cm3 g−1), and excellent thermodynamic stability (up to 600 °C). Benefiting from these advantages, OMCTs serving as the electrode materials for supercapacitor exhibited superior supercapacitor performances, including high capacitance of 247 F g−1 at 0.2 A g−1, satisfactory rate performance of 190 F g−1 at 5 A g−1, and cyclability.

Clinoatacamite (γ-Cu 2 (OH) 3 Cl) possesses a geometrically frustrated kagome lattice for the S = 1/2 antiferromagnetic spin system. Thus, it is deemed as the mother compound of many promising quantum spin liquid materials. Here, we synthesized clinoatacamite consisting of homogeneous octahedronlike particles with an average size of 1−2 μm via a hydrothermal strategy. Clinoatacamite crystallizes in a monoclinic lattice composed of Jahn−Teller distorted Cu(OH) 6 and Cu(OH) 4 Cl 2 octahedrons. The bonding nature of clinoatacamite is characterized using Raman scattering and FTIR absorption spectroscopies, which reveal the existence of trimeric hydrogen bonds. The magnetic measurements indicate that at temperatures below about 6 K, the magnetic response of the prepared samples is dominated by weak ferromagnetic contributions. The compression behavior is investigated by in situ high-pressure synchrotron radiation X-ray diffraction and Raman scattering spectroscopy. An isostructural phase transition is observed at about 8.4 GPa, which is evidenced by the anomalies in the variation curves of the lattice parameters and Raman scattering frequencies with pressure. The occurrence of the isostructural phase transition is attributed to the competition and cooperation of the external pressure and intrinsic Jahn−Teller effect, together with the interplay of intrastructural hydrogen bonding.

The Front Cover shows an interface‐induced self‐assembly strategy to synthesize ordered mesoporous carbon/Ti3C2Tx heterostructures with high specific surface area and excellent thermostability. The obtained samples combine the advantages of ordered mesoporous carbon and MXene and exhibit superior electrochemical performance. The presented strategy overcomes the disadvantages of MXene, such as stackable nature, low surface area, and poor thermostability, strongly promoting the application of porous MXene‐based heterostructures for supercapacitors. More information can be found in the Full Paper by Z. Liu, H. Xiong, et al.

The growth and design of hyperbranched hierarchical nanoarchitectures attract considerable current research enthusiasm in various scientific and technological fields, in which high porosity, large surface area and strong coupling between the subbranches, are expected. In this paper, the growth of hierarchical ZnOHF nanoarchitectures via a hydrothermal strategy is demonstrated. A variety of controllable morphologies with tunable degrees of branching, such as nanoparticles, nanorods, polypods, sheaf-and spherulite-like prickly hierarchical nanoarchitectures, can be obtained with the controlled regulation of the synthetic parameters including temperature, reaction time and solvent component. For the formation of ZnOHF hierarchical nanoarchitectures, the crystal splitting growth mechanism plays the dominant role, which is evidenced by the time-dependent morphological evolution. It is shown that the gas sensing properties of ZnOHF hyperbranched hierarchical nanoarchitectures may be closely correlated with their branching degrees. The half-sheaf-shaped ZnOHF nanoarchitecture exhibits the highest response for ethanol among some common hazardous volatile compounds.

Invited for this month′s cover is the group of Zhen‐An Qiao at the Jilin University. The image shows the application of 2D ordered mesoporous carbon/MXene heterostructures in supercapacitors. The Full Paper itself is available at 10.1002/cssc.202101374.