Design and Advanced Manufacturing of NU-1000 Metal-Organic Frameworks with Future Perspectives for Environmental and Renewable Energy Applications.

Metal-organic frameworks (MOFs) represent a relatively new family of materials that attract lots of attention thanks to their unique features such as hierarchical porosity, active metal centers, versatility of linkers/metal nodes, and large surface area. Among the extended list of MOFs, Zr-based-MOFs demonstrate comparably superior chemical and thermal stabilities, making them ideal candidates for energy and environmental applications. As a Zr-MOF, NU-1000 is first synthesized at Northwestern University. A comprehensive review of various approaches to the synthesis of NU-1000 MOFs for obtaining unique surface properties (e.g., diverse surface morphologies, large surface area, and particular pore size distribution) and their applications in the catalysis (electro-, and photo-catalysis), CO2 reduction, batteries, hydrogen storage, gas storage/separation, and other environmental fields are presented. The review further outlines the current challenges in the development of NU-1000 MOFs and their derivatives in practical applications, revealing areas for future investigation.

2D MXenes Nanosheets for Advanced Energy Conversion and Storage Devices: Recent Advances and Future Prospects.

Since the initial MXenes were discovered in 2011, several MXene compositions constructed using combinations of various transition metals have been developed. MXenes are ideal candidates for different applications in energy conversion and storage, because of their unique and interesting characteristics, which included good electrical conductivity, hydrophilicity, and simplicity of large-scale synthesis. Herein, we study the current developments in two-dimensional (2D) MXene nanosheets for energy storage and conversion technologies. First, we discuss the introduction to energy storage and conversion devices. Later, we emphasized on 2D MXenes and some specific properties of MXenes. Subsequently, research advances in MXene-based electrode materials for energy storage such as supercapacitors and rechargeable batteries is summarized. We provide the relevant energy storage processes, common challenges, and potential approaches to an acceptable solution for 2D MXene-based energy storage. In addition, recent advances for MXenes used in energy conversion devices like solar cells, fuel cells and catalysis is also summarized. Finally, the future prospective of growing MXene-based energy conversion and storage are highlighted.

The Emergence of 2D MXenes Based Zn-Ion Batteries: Recent Development and Prospects.

Rechargeable zinc-ion batteries (ZIBs) with exceptional theoretical capacity have garnered significant interest in large-scale electrochemical energy storage devices due to their low cost, abundant material, inherent safety, high specific energy, and ecofriendly nature. Metal carbides/nitrides, known as MXenes, have emerged as a large family of 2D transition metal carbides or carbonitrides with excellent properties, e.g., high electrical conductivity, large surface functional groups (e.g., F, O, and OH), low energy barriers for the diffusion of electrolyte ions with wide interlayer spaces. After a decade of effort, significant development has been achieved in the synthesis, properties, and applications of MXenes. Thus, it has opened up various exciting opportunities to construct advanced MXene-based nanostructures for ZIBs with excellent specific energy and power. Herein, this review summarizes the advances across multiple synthesis routes, related properties, morphological and structural characteristics, and chemistries of MXenes for ZIBs. The recent development of MXene-based electrodes is introduced, and electrolytes for ZIBs are elucidated in detail. MXene-based rocking chair ZIBs, strategies to enhance the performance of MXene-based cathodes, suppress the dendrites in MXene-based anodes, and MXene-based flexible ZIBs are pointed out. A rational design and modification of the MXenes as well as the production of composites with metal oxides exhibits promise in solving issues and enhancing the electrochemical performance of ZIBs. Finally, the present challenges and future prospects for MXene-based ZIBs are discussed.

Identification of Catalytic Active Sites for Durable Proton Exchange Membrane Fuel Cell: Catalytic Degradation and Poisoning Perspectives.

Recent progress in synthetic strategies, analysis techniques, and computational modeling assist researchers to develop more active catalysts including metallic clusters to single-atom active sites (SACs). Metal coordinated N-doped carbons (M-N-C) are the most auspicious, with a large number of atomic sites, markedly performing for a series of electrochemical reactions. This perspective sums up the latest innovative and computational comprehension, while giving credit to earlier/pioneering work in carbonaceous assembly materials towards robust electrocatalytic activity for proton exchange membrane fuel cells via inclusive performance assessment of the oxygen reduction reaction (ORR). M-Nx -Cy are exclusively defined active sites for ORR, so there is a unique possibility to intellectually design the relatively new catalysts with much improved activity, selectivity, and durability. Moreover, some SACs structures provide better performance in fuel cells testing with long-term durability. The efforts to understand the connection in SACs based M-Nx -Cy moieties and how these relate to catalytic ORR performance are also conveyed. Owing to comprehensive practical application in the field, this study has covered very encouraging aspects to the current durability status of M-N-C based catalysts for fuel cells followed by degradation mechanisms such as macro-, microdegradation, catalytic poisoning, and future challenges.

Recent Advances in Synthesis and Applications of Single-Atom Catalysts for Rechargeable Batteries.

The rapid development of flexible and wearable optoelectronic devices, demanding the superior, reliable, and ultra-long cycling energy storage systems. But poor performances of electrode materials used in energy devices are main obstacles. Recently, single-atom catalysts (SACs) are considered as emerging and potential candidates as electrode materials for battery devices. Herein, we have discussed the recent methods for the fabrication of SACs for rechargeable metal-air batteries, metal-CO2 batteries, metal-sulfur batteries, and other batteries, following the recent advances in assembling and performance of these batteries by using SACs as electrode materials. The role of SACs to solve the bottle-neck problems of these energy storage devices and future perspectives are also discussed.

Unprecedented Dual Role of Polyaniline for Enhanced Pseudocapacitance of Cobalt-Iron Layered Double Hydroxide.

Creating nanosized pores in layered materials can increase the abundant active surface area and boost potential applications of energy storage devices. Herein, a unique synthetic strategy based on polyaniline (PANI) doped 2D cobalt-iron layered double hydroxide (CoFe-LDH/P) nanomaterials are designed, and the formation of pores at low temperature (80 °C) is developed. It is found that the optimized concentration of PANI creates the nanopores on the CoFe-LDH nanosheets among all other polymers. The well-ordered pores of CoFe-LDH/P allow the high accessibility of the redox-active sites and promote effective ion diffusion. The optimized CoFe-LDH/P2 cathode reveals a specific capacitance 1686 (1096 Cg-1 ) and 1200 Fg-1 (720 Cg-1 ) at 1 and 30 Ag-1 respectively, a high rate capability (71.2%), and a long cycle life (98% over 10 000 cycles) for supercapacitor applications. Charge storage analysis suggests that the CoFe-LDH/P2 electrode displays a capacitive-type storage mechanism (69% capacitive at 1 mV s-1 ). Moreover, an asymmetric aqueous supercapacitor (CoFe-LDH/P2//AC) is fabricated, delivering excellent energy density (75.9 Wh kg-1 at 1124 W kg-1 ) with outstanding stability (97.5%) over 10 000 cycles. This work opens a new avenue for designing porous 2D materials at low temperature for aqueous energy storage devices.

Flower-like Highly Open-Structured Binder-Free Zn-Co-Oxide Nanosheet for High-Performance Supercapacitor Electrodes.

Scientific research is being compelled to develop highly efficient and cost-effective energy-storing devices such as supercapacitors (SCs). The practical use of SC devices is hindered by their low energy density and poor rate capability due to the binding agents in fabricating electrodes. Herein, we proposed flower-like highly open-structured binder-free ZnCo2O4 micro-flowers composed of nanosheets supported in nickel foam (ZnCoO@NF) with improved rate capability up to 91.8% when current varied from 2 to 20 A·g-1. The ZnCoO@NF electrode exhibited a superior specific capacitance of 1132 F·g-1 at 2 A·g-1 and revealed 99% cycling stability after 7000 cycles at a high current density of 20 A·g-1. The improved performance of the ZnCoO@NF electrode is attributed to the highly stable structure of the micro/nano-multiscale architecture, which provides both the high conduction of electrons and fast ionic transportation paths simultaneously.

A New MBH Adduct as an Efficient Ligand in the Synthesis of Metallodrugs: Characterization, Geometrical Optimization, XRD, Biological Activities, and Molecular Docking Studies.

This article reports the synthesis, characterization, geometrical optimization, and biological studies of new MBH-based organometallic compounds of medicinal significance. The ligand (MNHA) was prepared via the Morita-Baylis-Hillman (MBH) synthetic route, from aromatic aldehyde containing multiple functional groups. Metal complexes were prepared in an alkaline medium and under other suitable reaction conditions. Spectral and elemental analyses were used to identify the structural and molecular formulas of each compound. Optimized geometry was determined through density functional theory (DFT) B3LYP and 6-311++ G (d,p) basis set for the MBH adduct, whereas structures of novel complexes were optimized with the semi-empirical PM6 method. Powder XRD analysis furnished the crystal class of complexes, with Co3+, Cr3+, and Mn2+ being cubic, while Ni2+ was hexagonal, and Cu2+ was orthorhombic. Moreover, the ligand, along with Ni2+ and Co3+ complexes, showed profound antibacterial action against S. aureus, E. coli, B. pumilis, and S. typhi. Additionally, all of the complexes were shown to persist in the positive antioxidant potential of the ligand. Contrarily, not a single metal complex conserved the antifungal potentials of the ligand.

In Situ Nitrogen Functionalization of 2D-Ti3C2Tx-MXenes for High-Performance Zn-Ion Supercapacitor.

Zinc (Zn) ion supercapacitors (ZISCs) have attracted considerable attention as a viable energy storage technology because they are cost-effective, safe, and environmentally friendly. However, cathode materials with suitable properties are rare and need to be explored. In this regard, metal carbides (MXenes) are a good choice for capacitive energy storage, but they exhibit low capacitance. The energy storage performance of MXenes can be bossed using functionalization with heteroatom doping, e.g., nitrogen (N), to simultaneously modify ZISCs' fundamental characteristics and electrochemical properties. Herein, we present an in-situ N-functionalization of Ti3C2Tx-MXene via a hydrothermal reaction with urea (denoted as N-Ti3C2Tx-MXene). N-functionalization into Ti3C2Tx-MXene raised Ti3C2Tx-MXene's interlayer spacing and boosted the Zn-ion storage in 1 M ZnSO4 electrolyte. The N-Ti3C2Tx-MXene electrode delivered an excellent specific capacitance of 582.96 F/g at 1 A/g and retained an outstanding cycle stability of 94.62% after 5000 cycles at 10 A/g, which is 1.8 times higher than pristine Ti3C2Tx-MXene at identical conditions. Moreover, the N-Ti3C2Tx-MXene//Zn device demonstrated a maximum capacitance of 153.55 F/g at 1 A/g, retained 92% of its initial value after 5000 cycles, and its Coulombic efficiency was ~100%. This strategy considerably reduced Ti3C2Tx-MXene nanosheet restacking and aggregation and enhanced electrochemical performance. Further, this research elucidated N-Ti3C2Tx-MXene's charge-storage process and offered a fresh approach to the rational design of novel electrode materials for ZISCs.

SnS2nanosheet arrays anchoring on functionalized carbon cloth for quasi-solid-state flexible supercapacitor with satisfactory electrochemical performance and mechanical stability.

Increasing requirements for wearable devices stimulate the development of flexible energy storage components. Herein, a flexible integrated electrode consisting of SnS2nanosheet arraysin situanchored on the functionalized carbon cloth was prepared via a facile one-step hydrothermal method. Through pretreatment of carbon cloth, rough morphology is appeared on the surface of carbon fiber, which is conducive to optimizing the accessible load of SnS2. The SnS2nanosheet arrays and the carbon fiber as conductive skeleton cooperate with each other to provide a highly open surface, leading to the enhancement in capacitance (194.4 mF cm-2) and the outstanding retention after long-term service (86.5% after 10 000 cycles). A quasi-solid-state asymmetric flexible supercapacitor was assembled to evaluate the practical application under various conditions, suggesting satisfactory electrochemical performance as a maximum energy density of 10.95µWh cm-2at the power density of 4.75 mW cm-2and mechanical stability under actual conditions.

Energy storage properties of hydrothermally processed ultrathin 2D binder-free ZnCo2O4nanosheets.

High energy-density supercapacitors (SCs) with long operating life, cost-effective, and competitive cycling performance is attracted great research attention to competing in the requirements of the modern age. However, despite these benefits, SC hampers inadequate rate-capability and structural deterioration, which primarily affects its commercialization. Herein, ultra-thin two-dimensional (2D) ZnCo2O4nanosheets arein situanchored on the conductive surface of nickel foam (denoted as ZCO@NF) by hydrothermal process. The binder-free ZCO@NF is employed as an electrode for SCs and shows impressive charge storage properties. ZCO@NF electrode exhibited a high capacitance of 1250 (750) and 733 F g-1(440 C g-1) at 2.5 and 20 A g-1, respectively, demonstrating the outstanding rate-capability of 58.6% even at 8 times larger current density. Furthermore, the ZCO@NF electrode exhibits admirable capacitance retention of 96.5% after 10 000 cycles. This impressive performance of the ZCO@NF electrode is attributed to the high surface area which gives a short distance for ion/electron transfer, a high conductivity with extensive electroactive cities, and strong structural stability. The binder-free approach provides a strong relationship between the current collector and the active material, which turns into improved electrochemical operation as an electrode material for SCs.

Nanostructure Engineering of Metal-Organic Derived Frameworks: Cobalt Phosphide Embedded in Carbon Nanotubes as an Efficient ORR Catalyst.

Heteroatom doping is considered an efficient strategy when tuning the electronic and structural modulation of catalysts to achieve improved performance towards renewable energy applications. Herein, we synthesized a series of carbon-based hierarchical nanostructures through the controlled pyrolysis of Co-MOF (metal organic framework) precursors followed by in situ phosphidation. Two kinds of catalysts were prepared: metal nanoparticles embedded in carbon nanotubes, and metal nanoparticles dispersed on the carbon surface. The results proved that the metal nanoparticles embedded in carbon nanotubes exhibit enhanced ORR electrocatalytic performance, owed to the enriched catalytic sites and the mass transfer facilitating channels provided by the hierarchical porous structure of the carbon nanotubes. Furthermore, the phosphidation of the metal nanoparticles embedded in carbon nanotubes (P-Co-CNTs) increases the surface area and porosity, resulting in faster electron transfer, greater conductivity, and lower charge transfer resistance towards ORR pathways. The P-Co-CNT catalyst shows a half-wave potential of 0.887 V, a Tafel slope of 67 mV dec-1, and robust stability, which are comparatively better than the precious metal catalyst (Pt/C). Conclusively, this study delivers a novel path for designing multiple crystal phases with improved catalytic performance for energy devices.

Improved Electrochemical Performance of Aqueous Hybrid Supercapacitors Using CrCo2O4 Mesoporous Nanowires: An Innovative Strategy toward Sustainable Energy Devices.

High-rate aqueous hybrid supercapacitors (AHSCs) have attracted relevant scientific significance owing to their expected energy density, supercapacitor-level power density, and battery-level energy density. In this work, a bimetallic nanostructured material with chromium-incorporated cobalt oxide (CCO, i.e., CoCr2O4) was prepared via a hydrothermal method to form a stable cubic obelisk structure. Compared with CCO materials prepared using traditional methods, CCO displayed a nanowire structure (50 nm diameter), suggesting an enhanced specific surface area and a large number of active sites for chemical reactions. The electrode possessed a high specific capacitance (2951 F g-1) at a current density of 1 A g-1, minimum Rct (0.135 Ω), and the highest capacitance retention (98.7%), making it an ideal electrode material for AHSCs. Ex situ analysis based on X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) showed a favorable stability of CCO after 10,000 cycles without any phase changes being detected. GGA and GGA + U methods employed in density functional theory (DFT) also highlighted the enhanced metallic properties of CCO originating from the synergistic effect of semiconducting Cr2O3 and Co3O4 materials.

Biodegradable MoNx@Mo-foil electrodes for human-friendly supercapacitors.

With the advancement in the field of biomedical research, there is a growing demand for biodegradable electronic devices. Biodegradable supercapacitors (SCs) have emerged as an ideal solution for mitigating the risks associated with secondary surgeries, reducing patient discomfort, and promoting environmental sustainability. In this study, MoNx@Mo-foil was prepared as an active material for biodegradable supercapacitors through high-temperature and nitridation processes. The composite electrode exhibited superior electrochemical performance in both aqueous and solid-state electrolytes. In the case of the solid-state electrolyte, the MoNx@Mo-foil composite electrode-based device demonstrated excellent cycling stability and electrochemical performance. Additionally, the composite electrode exhibited rapid and complete biodegradability in a 3% H2O2 solution. Through detailed experimental analysis and performance testing, we verified the potential application of the MoNx@Mo-foil composite electrode in biodegradable supercapacitors. This work provides a new choice of degradable material for developing biomedical electronic devices.

Hexagon MXene based heterojunction interface with high ion adsorption and electron transfer efficiency for soft-package potassium-ions aqueous supercapacitors.

Potassium-ion hybrid capacitors (PIHC) are considered as ideal large-scale rechargeable energy storage devices due to their low-cost, high-power density and environmental protection. However, a low energy density is the main factor restricting the practical application of PIHC. The interface is formed on the surface of electrode material of PIHC through strong correlation to construct heterojunction, which can significantly improve the performance of ion energy storage. However, how to reveal the influence of the interfacial state of the heterojunction on the adsorption and electron transmission of energy storage ions at the atomic level is still one of the key scientific problems in this field. In this work, metal ion intercalation and microwave-assisted in-situ etching are used to construct the Hexagon MXene Ti3C2 heterojunction with TiOHO strong correlation. At the interface of heterojunction, TiOHO highway for electron transmission is developed to improve the rate performance of PIHC. Through experimental and theoretical calculation, the optimum adsorption position and maximum adsorption amount of potassium-ion at the single interface of heterojunction are obtained, and the specific energy density of PIHC is increased. This lays a foundation for the practical application of high-performance soft-package PIHC.

Recent trends in wastewater treatment by using metal-organic frameworks (MOFs) and their composites: A critical view-point.

Respecting the basic need of clean and safe water on earth for every individual, it is necessary to take auspicious steps for waste-water treatment. Recently, metal-organic frameworks (MOFs) are considered as promising material because of their intrinsic features including the porosity and high surface area. Further, structural tunability of MOFs by following the principles of reticular chemistry, the MOFs can be functionalized for the high adsorption performance as well as adsorptive removal of target materials. However, there are still some major concerns associated with MOFs limiting their commercialization as promising adsorbents for waste-water treatment. The cost, toxicity and regenerability are the major issues to be addressed for MOFs to get insightful results. In this article, we have concise the current strategies to enhance the adsorption capacity of MOFs during the water-treatment for the removal of toxic dyes, pharmaceuticals, and heavy metals. Further, we have also discussed the role of metallic nodes, linkers and associated functional groups for effective removal of toxic water pollutants. In addition to conformist overview, we have critically analyzed the MOFs as adsorbents in terms of toxicity, cost and regenerability. These factors are utmost important to address before commercialization of MOFs as adsorbents for water-treatment. Finally, some future perspectives are discussed to give directions for potential research.

V-MXenes for Energy Storage/Conversion Applications.

MXenes, a two-dimensional (2D) material, exhibit excellent optical, electrical, chemical, mechanical, and electrochemical properties. Titanium-based MXene (Ti-MXene) has been extensively studied and serves as the foundation for 2D MXenes. However, other transition metals possess the potential to offer excellent properties in various applications. This comprehensive review aims to provide an overview of the properties, challenges, key findings, and applications of less-explored vanadium-based MXenes (V-MXenes) and their composites. The current trends in V-MXene and their composites for energy storage and conversion applications have been thoroughly summarized. Overall, this review offers valuable insights, identifies potential opportunities, and provides key suggestions for future advancements in the MXenes and energy storage/conversion applications.

M4X3 MXenes: Application in Energy Storage Devices.

MXene has garnered widespread recognition in the scientific community due to its remarkable properties, including excellent thermal stability, high conductivity, good hydrophilicity and dispersibility, easy processability, tunable surface properties, and admirable flexibility. MXenes have been categorized into different families based on the number of M and X layers in Mn+1Xn, such as M2X, M3X2, M4X3, and, recently, M5X4. Among these families, M2X and M3X2, particularly Ti3C2, have been greatly explored while limited studies have been given to M5X4 MXene synthesis. Meanwhile, studies on the M4X3 MXene family have developed recently, hence, demanding a compilation of evaluated studies. Herein, this review provides a systematic overview of the latest advancements in M4X3 MXenes, focusing on their properties and applications in energy storage devices. The objective of this review is to provide guidance to researchers on fostering M4X3 MXene-based nanomaterials, not only for energy storage devices but also for broader applications.

Mo-based MXenes: Synthesis, properties, and applications.

Ti-MXene allows a range of possibilities to tune their compositional stoichiometry due to their electronic and electrochemical properties. Other than conventionally explored Ti-MXene, there have been ample opportunities for the non-Ti-based MXenes, especially the emerging Mo-based MXenes. Mo-MXenes are established to be remarkable with optoelectronic and electrochemical properties, tuned energy, catalysis, and sensing applications. In this timely review, we systematically discuss the various organized synthesis procedures, associated experimental tunning parameters, physiochemical properties, structural evaluation, stability challenges, key findings, and a wide range of applications of emerging Mo-MXene over Ti-MXenes. We also critically examined the precise control of Mo-MXenes to cater to advanced applications by comprehensively evaluating the summary of recent studies using artificial intelligence and machine learning tools. The critical future perspectives, significant challenges, and possible outlooks for successfully developing and using Mo-MXenes for various practical applications are highlighted.

Green synthesized Ag decorated CeO2 nanoparticles: Efficient photocatalysts and potential antibacterial agents.

Implication of natural resources for manufacturing of nanoparticles is sustainable, economical and contaminant free approach towards ecological and medical applications. Herein, CeO2 and Ag/CeO2 nanoparticles are green synthesized from Morinda tinctoria plant extract. The phase structure, surface morphology, optical identity, Ce(III) and Ce(IV) valency of the synthesized CeO2 and Ag/CeO2 nanoparticles are explored. The X-ray diffraction analysis indicated the formation of cubic phase CeO2 and cubic silver decorated CeO2 nanoparticles. Fourier transform infrared (FTIR) spectroscopy revealed the metal decoration of CeO2 nanoparticles, metal-oxygen stretching, indicating the plant molecules reduction and stabilization. UV-visible spectroscopy shown the decreased band gap owing to silver modification. Scanning electron microscopy (SEM) and transmission electron microscopy (TEM) micrographs displayed spherical morphology of the nanoparticles. Elemental composition and sample purity is assessed by energy dispersive spectroscopy (EDS). Double oxidation of Ce, double splitting energy of Ag and lattice oxygen are observed from X-ray photoelectron spectroscopy (XPS). Photocatalytic activity of Ag/CeO2 exposed the enhanced photocatalytic activity up to 94% where CeO2 nanoparticles gave 60% degradation of bromophenol blue (BB). The plasmonic decoration of silver on the ceria surface induced the charge separations and free radical reactions. Moreover, Ag/CeO2 nanoparticles are seen as superior antibacterial agents than CeO2 towards both E.coli and S.aureus. Hence, the silver decorated metal oxide photocatalyst successfully degraded the BB dye and inactivated the bacterial strains. This report established a future research in green synthesis of multipurpose metal nanoparticles.