Rapid detection of intact SARS-CoV-2 using designer DNA Nets and a pocket-size smartphone-linked fluorimeter.

Rapid, sensitive, and inexpensive point-of-care diagnosis is vital to controlling highly infectious diseases, including COVID-19. Here, we report the design and characterization of a compact fluorimeter called a "Virus Pod" (V-Pod) that enables sensitive self-testing of SARS-CoV-2 viral load in saliva. The rechargeable battery-operated device reads the fluorescence generated by Designer DNA Nanostructures (DDN) when they specifically interact with intact SARS-CoV-2 virions. DDNs are net-shaped self-assembling nucleic acid constructs that provide an array of highly specific aptamer-fluorescent quencher duplexes located at precise positions that match the pattern of spike proteins. The room-temperature assay is performed by mixing the test sample with DNA Net sensor in a conventional PCR tube and placing the tube into the V-Pod. Fluorescent signals are generated when multivalent aptamer-spike binding releases fluorescent quenchers, resulting in rapid (5-min) generation of dose-dependent output. The V-Pod instrument performs laser excitation, fluorescence intensity quantitation, and secure transmission of data to an App via Bluetooth™. We show that the V-Pod and DNA Net assay achieves clinically relevant detection limits of 3.92 × 103 viral-genome-copies/mL for pseudo-typed wild-type SARS-CoV-2 and 1.84 × 104, 9.69 × 104, 6.99 × 104 viral-genome-copies/mL for pathogenic Delta, Omicron, and D614G variants, representing sensitivity similar to laboratory-based PCR. The pocket-sized instrument (∼$294), inexpensive reagent-cost/test ($1.26), single-step, rapid sample-to-answer, and quantitative output represent a capability that is compatible with the needs of frequent self-testing in a consumer-friendly format that can link with medical service systems such as healthcare providers, contact tracing, and infectious disease reporting.

Template-Mediated Synthesis of Hierarchically Porous Metal-Organic Frameworks for Efficient CO2/N2 Separation.

Carbon dioxide (CO2) is generally unavoidable during the production of fuel gases such as hydrogen (H2) from steam reformation and syngas composed of carbon monoxide (CO) and hydrogen (H2). Efficient separation of CO2 from these gases is highly important to improve the energetic utilization efficiency and prevent poisoning during specific applications. Metal-organic frameworks (MOFs), featuring ordered porous frameworks, high surface areas and tunable pore structures, are emerging porous materials utilized as solid adsorbents for efficient CO2 capture and separation. Furthermore, the construction of hierarchical MOFs with micropores and mesopores could further promote the dynamic separation processes, accelerating the diffusion of gas flow and exposing more adsorptive pore surface. Herein, we report a simple, efficient, one-pot template-mediated strategy to fabricate a hierarchically porous CuBTC (CuBTC-Water, BTC = 1,3,5-benzenetricarboxylate) for CO2 separation, which demonstrates abundant mesopores and the superb dynamic separation ability of CO2/N2. Therefore, CuBTC-Water demonstrated a CO2 uptake of 180.529 cm3 g-1 at 273 K and 1 bar, and 94.147 cm3 g-1 at 298 K and 1 bar, with selectivity for CO2/N2 mixtures as high as 56.547 at 273 K, much higher than microporous CuBTC. This work opens up a novel avenue to facilely fabricate hierarchically porous MOFs through one-pot synthesis for efficient dynamic CO2 separation.

Puffing Up Hollow Carbon Nanofibers with High-Energy Metal-Organic Frameworks for Capacitive-Dominated Potassium-Ion Storage.

Nitrogen-doped carbon materials with abundant defects and strong potassium adsorption ability have been recognized as potential anodes for potassium ion batteries (PIBs). However, the limited content and uncontrolled type of nitrogen-doped sites hinder the further performance improvement of PIBs. Herein, this work proposes nitrogen phosphorous co-doped hollow carbon nanofibers (PNCNFs) derived from high-energy metal-organic frameworks (MOFs) with an ultra-high nitrogen content of 19.52 wt% and a high portion of more reactive pyridinic N sites. Furthermore, the highly open architecture exploded by released gases from high-energy MOFs provides sufficient edge sites to settle the N atoms and further form pyridinic N sites induced by phosphorous dopants. The resulting PNCNFs achieve excellent potassium ion storage performance with high reversible capacity (466.2 mAh g-1 ), superb rate capability (244.4 mAh g-1 at 8 A g-1 ), and excellent cycling performance (294.6 mAh g-1 after 3250 cycles). The density functional theory calculation reveals that the N/P defects enhance the potassium adsorption ability and improve the conductivity.

Tailoring Amine-Functionalized Ti-MOFs via a Mixed Ligands Strategy for High-Efficiency CO2 Capture.

Amine-functionalized metal-organic frameworks (MOFs) are a promising strategy for the high-efficiency capture and separation of CO2. In this work, by tuning the ratio of 1,3,5-benzenetricarboxylic acid (H3BTC) to 5-aminoisophthalic acid (5-NH2-H2IPA), we designed and synthesized a series of amine-functionalized highly stable Ti-based MOFs (named MIP-207-NH2-n, in which n represents 15%, 25%, 50%, 60%, and 100%). The structural analysis shows that the original framework of MIP-207 in the MIP-207-NH2-n (n = 15%, 25%, and 50%) MOFs remains intact when the mole ratio of ligand H3BTC to 5-NH2-H2IPA is less than 1 to 1 in the resulting MOFs. By the introduction of amino groups, MIP-207-NH2-25% demonstrates outstanding CO2 capture performance up to 3.96 and 2.91 mmol g-1, 20.7% and 43.3% higher than those of unmodified MIP-207 at 0 and 25 °C, respectively. Furthermore, the breakthrough experiment indicates that the dynamic CO2 adsorption capacity and CO2/N2 separation factors of MIP-207-NH2-25% are increased by about 25% and 15%, respectively. This work provides an additional strategy to construct amine-functionalized MOFs with the maintenance of the original MOF structure and high performance of CO2 capture and separation.

A Metal-Organic Framework Nanorod-Assembled Superstructure and Its Derivative: Unraveling the Fast Potassium Storage Mechanism in Nitrogen-Modified Micropores.

3D carbon-based materials with multiscale hierarchy are promising electrode materials for electrochemical energy storage and conversion applications, but the synthesis in an efficient and large-scale way is still a great challenge. Herein, a carbon nanorod-assembled 3D superstructure is facilely fabricated by morphology-preserving conversion of a metal-organic framework (MOF) nanorod-assembled superstructure. The MOF superstructure can be fabricated in one-pot synthesis with high reproducibility and high yield by precise control of the MOF nucleation and growth. Its derived carbon inherits the nanorod-assembled superstructure and possesses abundant micropores and nitrogen doping, which can serve as a high-performance anode material for fast potassium storage. The superiority of the superstructure and the synergism of micropore capturing and nitrogen anchoring are verified both experimentally and theoretically.

Pristine Hollow Metal-Organic Frameworks: Design, Synthesis and Application.

Metal-organic frameworks (MOFs), featuring porous crystalline structures with coordinated metal nodes and organic linkers, have recently found increasing interest in diverse applications. By virtue of their versatile and highly tunable compositions and structures, constructing hollow architectures will further endow MOFs with enhanced properties and designability, exceeding the molecular scale. MOFs could be considered as promising building units to fabricate complex hollow nanocomposites with faster mass transport, multiple active components, more exposed active sites, and better compatibility than bulk MOFs. To construct a promising blueprint for hollow pristine MOFs, this review provides a comprehensive overview for structural design strategies and applications of hollow pristine MOFs. We will highlight the merits, challenges and future potential by structuring and applying MOFs in sensing, separation, storage, catalysis, environmental remediation, photochemical and electrochemical energy conversion. This review might pave a new avenue for future development of novel pristine hollow MOFs.

Fabrication of Hollow CoP/TiOx Heterostructures for Enhanced Oxygen Evolution Reaction.

Transition-metal phosphides have flourished as promising candidates for oxygen evolution reaction (OER) electrocatalysts. Herein, it is demonstrated that the electrocatalytic OER performance of CoP can be greatly improved by constructing a hybrid CoP/TiOx heterostructure. The CoP/TiOx heterostructure is fabricated using metal-organic framework nanocrystals as templates, which leads to unique hollow structures and uniformly distributed CoP nanoparticles on TiOx . The strong interactions between CoP and TiOx in the CoP/TiOx heterostructure and the conductive nature of TiOx with Ti3+ sites endow the CoP-TiOx hybrid material with high OER activity comparable to the state-of-the-art IrO2 or RuO2 OER electrocatalysts. In combination with theoretical calculations, this work reveals that the formation of CoP/TiOx heterostructure can generate a pathway for facile electron transport and optimize the water adsorption energy, thus promoting the OER electrocatalysis.