General Synthesis Research Articles

A Universal Synthesis of Single-Atom Catalysts via Operando Bond Formation Driven by Electricity.

Single-atom catalysts (SACs), featuring highly uniform active sites, tunable coordination environments, and synergistic effects with support, have emerged as one of the most efficient catalysts for various reactions, particularly for electrochemical CO2 reduction (ECR). However, the scalability of SACs is restricted due to the limited choice of available support and problems that emerge when preparing SACs by thermal deposition. Here, an in situ reconstruction method for preparing SACs is developed with a variety of atomic sites, including nickel, cadmium, cobalt, and magnesium. Driven by electricity, different oxygen-containing metal precursors, such as MOF-74 and metal oxides, are directly atomized onto nitrogen-doped carbon (NC) supports, yielding SACs with variable metal active sites and coordination structures. The electrochemical force facilitates the in situ generation of bonds between the metal and the supports without the need for additional complex steps. A series of MNxOy (M denotes metal) SACs on NC have been synthesized and utilized for ECR. Among these, NiNxOy SACs using Ni-MOF-74 as a metal precursor exhibit excellent ECR performance. This universal and general SAC synthesis strategy at room temperature is simpler than most reported synthesis methods to date, providing practical guidance for the design of the next generation of high-performance SACs.

A General Enantioselective α-Alkyl Amino Acid Derivatives Synthesis Enabled by Cobalt-Catalyzed Reductive Addition.

Enantioenriched unnatural amino acids represent a prevalent motif in organic chemistry, with profound applications in biochemistry, medicinal chemistry, and materials science. Herein, we report a cobalt-catalyzed aza-Barbier reaction of dehydroglycines with unactivated alkyl halides to afford unnatural α-amino esters with high enantioselectivity. This catalytic reductive alkylative addition protocol circumvents the use of moisture-, air-sensitive organometallic reagents, and stoichiometric chiral auxiliaries, enabling the conversion of a variety of primary, secondary, and even tertiary unactivated alkyl halides to α-alkyl-amino esters under mild conditions, thus leading to broad functional group tolerance. The expedient access to biologically active motifs demonstrates the practicality of this protocol by reducing the number of synthetic steps and enhancing the reaction efficiency.

Understanding the Contributions of the Hippocampus

The hippocampus plays an important role in human memory, with its anterior portion contributing to coarse-grained representations and its posterior portion contributing to fine-grained ones (Poppenk et al., 2013). My USRA project is focused on understanding the role of the hippocampus in a potential third type of memory representation; a general synthesis of stimuli. Beyond memory, the hippocampus has also been hypothesize to influence clinical disorders. For instance, preliminary research in our lab has found meta-cognitive memory abilities to be organized into factors resembling clinical disorders, when organized by variance in brain structure. My USRA project also aims to understand the contribution of the hippocampus to clinical disorders. My role in this project has been to develop administrative and experimental structure for the protocol, which involves extensive testing. Participants will complete approximately 27 hours of memory tasks, designed to evaluate the nature of their memory, and whether it is oriented towards detail, gist, or a synthesis of all stimuli. To do so, I have developed an extensive task of reading and evaluating reviews, as well as a recall task of lab-generated stories. Participants will also complete approximately 3-4 hours of online questionnaires, administered through Qualtrics. Over the summer, I conducted research to identify validated questionnaires that assess metacognitive abilities, in the domains of memory, attention, language, motor control, social cognition and perception. Results on these questionnaires will be used to validate preliminary findings on the relationship between metacognitive memory, brain variance and sub-threshold levels of clinical disorders, and to investigate whether these findings expand to other forms of metacognition. Finally, participants will complete a number of structural and functional MRI scans (including DTI). This work may help us understand the pure science of the function of human memory, as well as the nature of clinical disorders.

On the synthesis and formability of high-entropy oxides

This paper reports on a straightforward and general solution-based synthesis method for high-entropy oxides (HEOs) of different types and compositions. The flexibility and simplicity of this method are hoped to drive development of new HEOs and study of their properties and applications. Thirteen HEOs with rock salt, fluorite, spinel, and perovskite structures were synthesized using a Pechini-type synthesis at temperatures significantly lower than those necessary in solid-state synthesis (400–900 °C). Metal nitrates, nitrites, chlorides, and even water-sensitive alkoxides were used as the metal precursors with the present method. The HEOs were characterized using powder X-ray diffraction, scanning electron microscopy, and energy-dispersive X-ray spectroscopy. Relaxation of cation size and charge rules and formability of HEOs are also discussed. The present results indicate that the classical criteria for material stability do not readily translate to high-entropy systems. For example, the well-known criteria for Goldschmidt and octahedral tolerance factors established for ordinary perovskites do not seem to describe formability of perovskite HEOs well. The discussed relaxation of cation size and charge rules will contribute to the understanding of HEO systems and development of new HEO phases.

General synthesis of porous metal oxides nanosheets for gas sensing by gradient crystallization induced spatial confinement approach

Inorganic-template synthesis of crystalline porous metal oxides nanosheets with fantastic properties is a powerful approach, but it is limited in the systems with strong interaction between inorganic crystals and guest species. Here, we report a gradient crystallization induced spatial confinement method to achieve a general synthesis of porous metal oxides nanosheets regardless of host–guest interaction. Taking the synthesis of porous SnO2 nanosheets as an example, the freezing of KCl/SnCl2 aqueous solution induces the gradient crystallization of lamellar ice and KCl structure, and subsequently expelled KCl/SnCl2 crystals can be limited in the confined region to form the ice/SnCl2/KCl sandwich structure. Followed by freeze-drying, calcination and water washing, the porous SnO2 nanosheets structure can be obtained. Notably, this general method enables the synthesis of functional porous nanosheet with specific designed component and surface properties, and the obtained porous Pt-SnO2 nanosheets with abundant accessible active sites and lower d-band center exhibit superior gas sensing performance to 3-hydroxy-2-butanone.

Arylboronic Acid Pinacol Esters as Stable Boron Sources for Dihydrodibenzoborepin Derivatives and a Dibenzoborole.

The general synthesis of boron-containing cyclic compounds (boracycles) necessitates toxic organotin precursors or highly reactive boron halides. Here, we report the synthesis of seven- and five-membered boracycles utilizing arylboronic acid pinacol esters (ArBpins) as stable boron sources. Grignard reagents generated from 2,2'-dibromodibenzyl or 2,2'-dibromobiphenyl reacted with ArBpins, where Ar = 9-anthryl (Anth), 2,4,6-trimethylphenyl (Mes), or 2,4,6-triisopropylphenyl (Tip), to give 10,11-dihydro-5H-dibenzo[b,f]borepins or dibenzoborole derivatives. This Bpin-based method was successfully applied to a one-shot double boracycle formation, providing a dihydrodibenzoborepin-anthracene-dihydrodibenzoborepin triad molecule in a good yield. The dihydrodibenzoborepin bearing the Anth group was directly converted to the unsaturated borepin by NBS/AIBN. All products were characterized by NMR, HRMS, and in some cases, single-crystal X-ray diffraction analysis. Additionally, the photophysical properties of the products are also reported.

General synthesis of high-entropy single-atom nanocages for electrosynthesis of ammonia from nitrate

Given the growing emphasis on energy efficiency, environmental sustainability, and agricultural demand, there’s a pressing need for decentralized and scalable ammonia production. Converting nitrate ions electrochemically, which are commonly found in industrial wastewater and polluted groundwater, into ammonia offers a viable approach for both wastewater treatment and ammonia production yet limited by low producibility and scalability. Here we report a versatile and scalable solution-phase synthesis of high-entropy single-atom nanocages (HESA NCs) in which Fe and other five metals-Co, Cu, Zn, Cd, and In-are isolated via cyano-bridges and coordinated with C and N, respectively. Incorporating and isolating the five metals into the matrix of Fe resulted in Fe-C5 active sites with a minimized symmetry of lattice as well as facilitated water dissociation and thus hydrogenation process. As a result, the Fe-HESA NCs exhibited a high selectivity toward NH3 from the electrocatalytic reduction of nitrate with a Faradaic efficiency of 93.4% while maintaining a high yield rate of 81.4 mg h−1 mg−1.

Revealing Enhanced Optical Nonlinearity and Robust Ferromagnetism in Atomically Sharp Stacking Binary-Ternary Magnetic Heterostructures.

Two-dimensional (2D) materials provide a versatile platform for the integration of diverse crystals, enabling the formation of heterostructures with intriguing functionalities. Coherently growing 2D heterostructures are highly desirable for property manipulation due to their strong interfacial interaction. In this work, we propose a general synthesis approach and provide insight into well-designed 2D binary-ternary magnetic heterostructures. Atomically sharp interfaces were achieved in typical lateral and vertical Cr1+mSe2(001)/CuCr2Se4(111) heterostructures owing to their similar lattice arrangement, with the observation of a significant enhancement of optical second-harmonic generation. Further magnetism measurements revealed a Curie temperature up to 360 K and thickness- and temperature-dependent magnetism in this heterostructure. Additionally, we synthesized three analogous 2D magnetic heterostructures in Fe-Cr-S, Co-Cr-S, and Cu-Cr-S systems, demonstrating the ubiquitous nature of the coherent heteroepitaxy. Our work involves the development of an innovative platform for investigating the underlying physics and potential applications of 2D binary-ternary heterostructures as well as the fabrication of associated functional devices.

Flash-within-flash synthesis of gram-scale solid-state materials.

Sustainable manufacturing that prioritizes energy efficiency, minimal water use, scalability and the ability to generate diverse materials is essential to advance inorganic materials production while maintaining environmental consciousness. However, current manufacturing practices are not yet equipped to fully meet these requirements. Here we describe a flash-within-flash Joule heating (FWF) technique-a non-equilibrium, ultrafast heat conduction method-to prepare ten transition metal dichalcogenides, three group XIV dichalcogenides and nine non-transition metal dichalcogenide materials, each in under 5 s while in ambient conditions. FWF achieves enormous advantages in facile gram scalability and in sustainable manufacturing criteria when compared with other synthesis methods. Also, FWF allows the production of phase-selective and single-crystalline bulk powders, a phenomenon rarely observed by any other synthesis method. Furthermore, FWF MoSe2 outperformed commercially available MoSe2 in tribology, showcasing the quality of FWF materials. The capability for atom substitution and doping further highlights the versatility of FWF as a general bulk inorganic materials synthesis protocol.

Development of Iron‐Based Single Atom Materials for General and Efficient Synthesis of Amines

AbstractEarth abundant metal‐based heterogeneous catalysts with highly active and at the same time stable isolated metal sites constitute a key factor for the advancement of sustainable and cost‐effective chemical synthesis. In particular, the development of more practical, and durable iron‐based materials is of central interest for organic synthesis, especially for the preparation of chemical products related to life science applications. Here, we report the preparation of Fe‐single atom catalysts (Fe‐SACs) entrapped in N‐doped mesoporous carbon support with unprecedented potential in the preparation of different kinds of amines, which represent privileged class of organic compounds and find increasing application in daily life. The optimal Fe‐SACs allow for the reductive amination of a broad range of aldehydes and ketones with ammonia and amines to produce diverse primary, secondary, and tertiary amines including N‐methylated products as well as drugs, agrochemicals, and other biomolecules (amino acid esters and amides) utilizing green hydrogen.

Development of Iron-Based Single Atom Materials for General and Efficient Synthesis of Amines.

Earth abundant metal-based heterogeneous catalysts with highly active and at the same time stable isolated metal sites constitute a key factor for the advancement of sustainable and cost-effective chemical synthesis. In particular, the development of more practical, and durable iron-based materials is of central interest for organic synthesis, especially for the preparation of chemical products related to life science applications. Here, we report the preparation of Fe-single atom catalysts (Fe-SACs) entrapped in N-doped mesoporous carbon support with unprecedented potential in the preparation of different kinds of amines, which represent privileged class of organic compounds and find increasing application in daily life. The optimal Fe-SACs allow for the reductive amination of a broad range of aldehydes and ketones with ammonia and amines to produce diverse primary, secondary, and tertiary amines including N-methylated products as well as drugs, agrochemicals, and other biomolecules (amino acid esters and amides) utilizing green hydrogen.

5 A Phase 1b, Open-Label, Safety, Tolerability, and Efficacy Study of HC-7366 in Combination with Belzutifan (WELIREGTM) in Patients with Advanced or Metastatic Renal Cell Carcinoma, NCT06234605

Abstract Background HC-7366 is a novel, orally administered, highly selective and potent activator of general control nonderepressible 2 (GCN2) kinase, a core regulator of metabolic stress through activation of the integrated stress response (ISR). Activation of GCN2 promotes cell survival, whereas prolonged activation induces apoptosis. GCN2 activation also suppresses general protein synthesis and induces cell cycle arrest, thereby preventing cell growth during nutrient scarcity. Additionally, HC-7366 decreases HIF expression and inhibits glycolysis, oxidative phosphorylation, and TCA cycle function. HC-7366 also inhibits HIF expression in immunosuppressive myeloid cells, including macrophages. These effects of HC-7366 on metabolism, HIF signaling, and immune suppression suggest therapeutic benefit in ccRCC with clear rationale for combinations with HIF2a antagonists and immune checkpoint inhibitors. HC-7366 (0.5-1 mg/kg), combined with belzutifan (1 mg/kg), exhibited combination benefit in HIF-2 dependent A-498 and 786-O RCC xenografts, yielding 90% tumor growth inhibition and a three-fold increase in complete responses, respectively. Additionally, HC-7366 drives significant monotherapy antitumor activity in PDX models that demonstrated belzutifan resistance. Mechanism of action studies have identified several pathway engagement and potential efficacy biomarkers (Stokes, et al., 2024). Trial design/schema This multicenter, open-label phase 1b study will identify the Maximum Tolerated Dose (MTD) and/or the Recommended Phase 2 Dose (RP2D) of HC-7366 in combination with fixed-dose belzutifan, 120 mg po qd, in patients with advanced or metastatic RCC with renal cell histology irrespective of VHL gene mutation. Monotherapy HC-7366 will be evaluated in parallel. The monotherapy arm, HC-7366, 60 mg p.o. qd, includes patients who have relapsed after 1 to 4 prior lines of standard of care that may include belzutifan or another HIF-2α inhibitor. The combination arm includes patients who have received 1 to 3 prior lines of standard of care and are belzutifan or HIF-2α naïve. HC-7366 dose escalation arm evaluates combination fixed dose belzutifan, 120 mg po qd plus HC-7366 at 20, 40, or 60 mg po qd. Enrollment will start with the HC-7366 monotherapy arm. Subsequently, patients will begin to enroll in the combination therapy HC-7366 dose escalation arm, while the monotherapy arm will continue to enroll. Expansion will evaluate the combination of fixed dose belzutifan with two doses of HC-7366 selected from escalation. Assessments include safety, PK, and anti-tumor activity. The study will enroll up to 80 patients at US study sites. Significance and vision Combination HC-7366 plus belzutifan, supported by preclinical evidence, is being studied to assess antitumor activity in the RCC relapsed setting. Determining safety and evaluation of dose are foundational to this study. Reference Stokes M, Tameire F, Wojnarowicz P, et al. HC-7366, a potent GCN2 activator, complements belzutifan, a HIF-2⍺ antagonist, by providing combination benefit in belzutifan-sensitive models and monotherapy activity in belzutifan-resistant models. Meeting of the American Association for Cancer Research; 2024 Apr 5-10; San Diego (CA); AACR; 2024. Abstract 4615. This study is in collaboration with Merck Sharp & Dohme LLC, a subsidiary of Merck & Co., Inc., Rahway, NJ, USA

Strategies for developing hard skills in higher education students through innovative pedagogical technologies in realistic professional environments

Introduction: the global emphasis on developing hard skills, essential for professional competence in digital optimization, has led to a focus on practical skills like foreign language proficiency, programming, and data analysis. These skills, acquired through education or experience, are crucial across various professions, especially in the digital era, where innovative pedagogical methods are key.Objectives: this study aims to analyze the impact of innovative pedagogical technologies on developing hard skills, particularly foreign language competence, in higher education students, simulating real-world professional environments.Methods: the study employs a range of general scientific methods, including analysis, synthesis, induction, deduction, formalization, and generalization. These methods help identify and describe the development of hard skills and digital competence, focusing on innovative pedagogical strategies.Results: the findings highlight a structural-functional model for professional training in the digital labor market, emphasizing interdisciplinary integration, professional training alignment with market needs, and the use of innovative technologies. Key skills identified include financial management, software development, and foreign language proficiency, essential for making informed managerial decisions in a globalized world.Conclusions: the integration of innovative pedagogical methods, such as incidental learning and argumentation, enhances the development of hard skills, particularly English language competence. The study underscores the importance of creating learning environments that closely mirror professional conditions, thereby improving the quality of education and preparing students for the demands of the modern labor market. Future research should focus on refining digital tools and methodologies to further enhance language skills and overall hard skill development

Synergy of social and institutional transformations in higher education in the context of post-war recovery: foreign experience for Ukraine

Introduction: the strategic directions for post-war recovery in Ukraine involve preserving and enhancing higher education institutions' educational and cultural potential, intensifying knowledge-intensive technologies' development, and transforming the education system towards public management and digitalisation. There is a growing demand for the development of higher education in productive educational-cognitive directions, specialisation, and universalisation. The article aims to analyse the potential synergy of the transformation of institutional and social concepts in the functioning of higher education in the context of post-war recovery in Ukraine. Method: the study employed general research methods, including generalisation, comparison, systematisation, abstraction, analysis, synthesis, and concretisation, to analyse the experience of foreign countries in adapting their higher education systems to crisis and post-crisis conditions. Results: the study examined the requirements and possibilities for modernising and improving the higher education system in Ukraine through the interaction between the labour market and the educational environment. The research summarised the issues with the functioning of the higher education system during martial law. It proposed a comprehensive approach to regenerating and optimising the higher education system during the post-war recovery period. Conclusions: the study demonstrated the need for synergy between social and institutional dynamics in higher education transformation. The results suggest ways to improve higher education by integrating different vectors of the social-institutional environment

Abstract Or113: Identification of Newly Synthesized Protein in Cardiomyocytes after Myocardial Infarction

Compared to mRNA, proteins perform ultimate functions in the heart and can be rapidly upregulated or downregulated in response to environmental inputs. Identifying how the proteome is altered in cardiomyocytes (CMs) after myocardial infarction (MI) will improve our understanding of the stress response signaling after MI and contribute to developing new therapeutic strategies. Here, we developed a method for determining which proteins in CMs are newly synthesized after MI by using mice expressing a mutant methionyl-tRNA synthetase that incorporates the non-canonical amino acid azidonorleucine into the newly synthesized peptides of CMs. We found that the proteins synthesized at the highest levels in homeostasis are involved in sarcomere structure and metabolism, which aligns with immunofluorescence staining results that showed enrichment of newly synthesized proteins localized at the sarcomere and intercalated disc. We showed that α-actin, a critical component of the sarcomere, and glyceraldehyde-3-phosphate dehydrogenase (GAPDH), an enzyme for glucose metabolism, are highly dynamic and require constant protein synthesis for maintenance. After MI, protein synthesis in CMs within the infarct area is halted, and the border zone CMs showed reduced protein synthesis. Most notably, proteins associated with mitochondrial oxidative phosphorylation are reduced compared with sham. By integrating with spatial transcriptomics, we also discovered that the MI-induced genes are enriched in CMs within the infarcted areas. These CMs exhibit decreased general protein synthesis, indicating a decoupling of transcriptional and translational regulation following MI. Collectively, our findings revealed that CMs rapidly respond to injuries by controlling protein synthesis, which is independent of the expression of mRNAs.

2D PtRhPb Mesoporous Nanosheets with Surface-Clean Active Sites for Complete Ethanol Oxidation Electrocatalysis.

The development of active and selective metal electrocatalysts for complete ethanol oxidation reaction (EOR) into desired C1 products is extremely promising for practical application of direct ethanol fuel cells. Despite some encouraging achievements, their activity and selectivity remain unsatisfactory. In this work, it is reported that 2D PtRhPb mesoporous nanosheets (MNSs) with anisotropic structure and surface-clean metal siteperform perfectly for complete EOR electrocatalysis in both three-electrode and two-electrode systems. Different to the traditional routes, a selective etching strategy is developed to produce surface-clean mesopores while retaining parent anisotropy quasi-single-crystalline structure without the mesopore-forming surfactants. This method also allows the general synthesis of surface-clean mesoporous metals with other compositions and structures. When being performed for alkaline EOR electrocatalysis, the best PtRhPb MNSs deliver remarkably high activity (7.8 A mg-1) and superior C1 product selectivity (70% of Faradaic efficiency), both of which are much better than reported electrocatalysts. High performance is assigned to multiple structural and compositional synergies that not only stabilized key OHads intermediate by surface-clean mesopores but also separated the chemisorption of two carbons in ethanol by adjacent Pt and Rh sites, which facilitate the oxidation cleavage of stable C─C bond for complete EOR electrocatalysis.

Deep learning-based general beam synthesis for atmospheric propagation

Optimizing the transmit light beams unlocks the full potential of free-space optical systems. However, designing application-specific light beams remains a challenge, especially for those traversing random media. In this study, we address this gap by proposing a deep learning-based method to generate optimal beams for propagation through atmospheric turbulence. The key mechanism is approximating the receiver statistics through batch-wise computation during the training of a convolutional neural network (CNN). On that basis, statistical performance metrics including average received power, scintillation index, and mean signal-to-noise ratio (SNR) are considered for optimization. Pseudo-modes of the beam are synthesized by weighted superposition of Hermite-Gaussian eigenmodes, enabling the creation of arbitrary complex amplitude profiles, i.e., general beams. An end-to-end implementation framework is designed to facilitate self-supervised learning and eliminate the need for pre-calculated datasets. Effectiveness of the synthesized beam is validated by wave optics simulation and experiments. In particular, comparison with Gaussian Schell-model beams demonstrates that the synthesized beam can achieve lower scintillation and greater intensity at the same time, leading to markedly enhanced receiver SNR. This advantage persists in a wider range of link configurations, extending the application range of stochastic beams.

Bismuth(III)-Catalyzed Regioselective Selenation of Indoles with Diaryl Diselenides: Synthesis of 3-Selanylindoles.

Heterocyclic aryl selenides have recently attracted considerable research interest owing to their applications in biological and pharmaceutical fields. Herein, we describe a simple and general synthesis of 3-selanylindoles via a novel regioselective C-H selenation of indoles using a bismuth reagent as a catalyst. The reactions of indoles with diselenides in the presence of 10 mol% BiI3 at 100 °C in DMF afforded the corresponding 3-selanylindoles in moderate-to-excellent yields. The reaction proceeded efficiently under aerobic conditions by adding only a catalytic amount of BiI3, which was non-hygroscopic and less toxic, and both selanyl groups of the diselenide were transferred to the desired products.

Disentangling the drivers of urban bird diversity in the non-breeding season: A general synthesis.

Current knowledge about the impacts of urbanisation on bird assemblages is based on evidence from studies partly or wholly undertaken in the breeding season. In comparison, the non-breeding season remains little studied, despite the fact that winter conditions at higher latitudes are changing more rapidly than other seasons. During the non-breeding season, cities may attract or retain bird species because they offer milder conditions or better feeding opportunities than surrounding habitats. However, the range of climatic, ecological and anthropogenic mechanisms shaping different facets of urban bird diversity in the non-breeding season are poorly understood. We explored these mechanisms using structural equation modelling to assess how urbanisation affects the taxonomic, phylogenetic and functional diversity of avian assemblages sampled worldwide in the non-breeding season. We found that minimum temperature, elevation, urban area and city age played a critical role in determining taxonomic diversity while a range of factors-including productivity, precipitation, elevation, distance to coasts and rivers, socio-economic (as a proxy of human facilitation) and road density-each contributed to patterns of phylogenetic and functional diversity. The structure and function of urban bird assemblages appear to be predominantly shaped by temperature, productivity and city age, with effects of these factors differing across seasons. Our results underline the importance of considering multiple hypotheses, including seasonal effects, when evaluating the impacts of urbanisation on biodiversity.

"Hard" Emulsion-Induced Interface Super-Assembly: A General Strategy for Two-Dimensional Hierarchically Porous Metal-Organic Framework Nanoarchitectures.

Two-dimensional (2D) hierarchically porous metal-organic framework (MOF) nanoarchitectures with tailorable meso-/macropores hold great promise for enhancing mass transfer kinetics, augmenting accessible active sites, and thereby boosting performance in heterogeneous catalysis. However, achieving the general synthesis of 2D free-standing MOF nanosheets with controllable hierarchical porosity and thickness remains a challenging task. Herein, we present an ingenious "hard" emulsion-induced interface super-assembly strategy for preparing 2D hierarchically porous UiO-66-NH2 nanosheets with highly accessible pore channels, tunable meso-/macropore sizes, and adjustable thicknesses. The methodology relies on transforming the geometric shape of oil droplet templates within appropriate oil-in-water emulsions from conventional zero-dimensional (0D) "soft" liquid spheres to 2D "hard" solid sheets below the oil's melting/freezing point. Subsequent surfactant exchange on the surface of 2D "hard" emulsions facilitates the heterogeneous nucleation and interfacial super-assembly of in situ formed mesostructured MOF nanocomposites, serving as structural units, in a loosely packed manner to produce 2D MOF nanosheets with multimodal micro/meso-/macroporous systems. Importantly, this strategy can be extended to prepare other 2D hierarchically porous MOF nanosheets by altering metal-oxo clusters and organic ligands. Benefiting from fast mass transfer and highly accessible Lewis acidic sites, the resultant 2D hierarchically porous UiO-66-NH2 nanosheets deliver a fabulous catalytic yield of approximately 96% on the CO2 cycloaddition of glycidyl-2-methylphenyl ether, far exceeding the yield of approximately 29% achieved using conventional UiO-66-NH2 microporous crystals. This "hard" emulsion-induced interface super-assembly strategy paves a new path toward the rational construction of elaborate 2D nanoarchitecture of hierarchical MOFs with tailored physicochemical properties for diverse potential applications.