Proximity-Induced Bipedal DNA Walker for Accurately Visualizing microRNA in Living Cancer Cell.

DNA walker, a type of dynamic DNA device that is capable of moving progressively along prescribed walking tracks, has emerged as an ideal and powerful tool for biosensing and bioimaging. However, most of the reported three-dimensional (3D) DNA walker were merely designed for the detection of a single target, and they were not capable of achieving universal applicability. Herein, we reported for the first time the development of a proximity-induced 3D bipedal DNA walker for imaging of low abundance biomolecules. As a proof of concept, miRNA-34a, a biomarker of breast cancer, is chosen as the model system to demonstrate this approach. In our design, the 3D bipedal DNA walker can be generated only by the specific recognition of two proximity probes for miRNA-34a. Meanwhile, it stochastically and autonomously traveled on 3D tracks (gold nanoparticles) via catalytic hairpin assembly (CHA), resulting in the amplified fluorescence signal. In comparison with some conventional DNA walkers that were utilized for living cell imaging, the 3D DNA walkers induced by proximity ligation assay can greatly improve and ensure the high selectivity of bioanalysis. By taking advantage of these unique features, the proximity-induced 3D bipedal DNA walker successfully realizes accurate and effective monitoring of target miRNA-34a expression levels in living cells, affording a universal, valuable, and promising platform for low-abundance cancer biomarker detection and accurate identification of cancer.

Anaerobic granular sludge performance in an expanded granular sludge bed reactor treating calcium-rich wastewater by adjusting CaCO3 crystallization: Effect of upflow velocity and Ca2+ concentration.

The role of upflow velocity and Ca2+ concentration in controlling the type and rate of CaCO3 crystallization and their impacts on the anaerobic granular sludge (AnGS) formation and performance in an expanded granular sludge bed (EGSB) reactor were studied. The results showed that an improved upflow velocity could promote metastable CaCO3 crystals and achieve the optimized portion of vaterite with a value of 84 % at 10 m/h with a small amount of aragonite, thus limiting the scaling in the reactor. The removal efficiency of Ca2+ was to some extent positively correlated to the influent Ca2+ concentration, but declined when Ca2+ exceeded a specific threshold. Vaterite was dominant with the increase of Ca2+ concentrations of the influent. Compared with granules in R1 (Ca2+ 10 mg/L) and R2 (Ca2+ 100 mg/L), granules cultivated in R3 (Ca2+ 800 mg/L) revealed maximum amount of biomass with biggest particle size distribution and fastest average settling rate, with relative stable COD removal efficiency and the fast optimized reactor capacity at OLR of 16 kgCOD/m3d. A low upflow velocity and a higher Ca2+ concentration promoted nucleus formation and granules growth at the initial cultivation stage of the EGSB reactor. The Ca2+ concentration had a significant impact on the bacterial community and favoured the growth of Tolumonas and Anaeromousa Anaeroarcus. Archaea, rather than bacteria, was strengthened to contribute more to methane production at a relatively high Ca2+ concentration.

Dialkylamines Driven Two-Step Recovery of NiOx/ITO Substrates for High-Reproducibility Recycling of Perovskite Solar Cells.

Because of the toxicity of water-soluble lead, the recycling of organic-inorganic lead-halides perovskite solar cells (PSCs) has attracted increasing attention. Here, we report a highly reliable two-step process to recycle cost-dominated indium-tin-oxide (ITO) substrates coated with NiOx and regenerate their based PSCs by function of dialkylamines. The champion recycled PSC can achieve 20% in conversion-efficiency, higher than 17.92% of the fresh one. Strikingly, the regenerated devices can remain superior to the fresh ones in the first 7 of 10 recycles. The comprehensive X-ray photoelectronic spectroscopy analysis reveals that dipropylamine has a suitable interaction with NiOx surfaces by Ni-N coordination, enabling its effective interfacial passivation and template effect of high-quality growth of perovskites. That leads to the suppressed nonradiative recombination of both interfacial and bulk, and finally improves the device performances. The dialkylamines driven two-step recycling process offers a promising and highly reproducible strategy to recycle PSCs, especially the cost-dominated NiOx/ITO substrates.

Teaching an Old Anchoring Group New Tricks: Enabling Low-Cost, Eco-Friendly Hole-Transporting Materials for Efficient and Stable Perovskite Solar Cells.

As a key component in perovskite solar cells (PVSCs), hole-transporting materials (HTMs) have been extensively explored and studied. Aiming to meet the requirements for future commercialization of PVSCs, HTMs which can enable excellent device performance with low cost and eco-friendly processability are urgently needed but rarely reported. In this work, a traditional anchoring group (2-cyanoacrylic acid) widely used in molecules for dye-sensitized solar cells is incorporated into donor-acceptor-type HTMs to afford MPA-BT-CA, which enables effective regulation of the frontier molecular orbital energy levels, interfacial modification of an ITO electrode, efficient defect passivation toward the perovskite layer, and more importantly alcohol solubility. Consequently, inverted PVSCs with this low-cost HTM exhibit excellent device performance with a remarkable power conversion efficiency (PCE) of 21.24% and good long-term stability in ambient conditions. More encouragingly, when processing MPA-BT-CA films with the green solvent ethanol, the corresponding PVSCs also deliver a substantial PCE as high as 20.52% with negligible hysteresis. Such molecular design of anchoring group-based materials represents great progress for developing efficient HTMs which combine the advantages of low cost, eco-friendly processability, and high performance. We believe that such design strategy will pave a new path for the exploration of highly efficient HTMs applicable to commercialization of PVSCs.

Side-Chain Engineering of Donor-Acceptor Conjugated Small Molecules As Dopant-Free Hole-Transport Materials for Efficient Normal Planar Perovskite Solar Cells.

Simultaneously improving efficiency and stability, which are particularly crucial factors for the commercialization of perovskite solar cells (PSCs), remains a major challenge. For high-efficiency normal PSCs, the development of stable dopant-free hole-transport materials (HTMs) seems imperative. Here, we developed potential donor-acceptor small molecules (BTTI) as HTMs for normal planar PSCs. Through tailoring its alkyl side-chain length as BTTI-C6, BTTI-C8, and BTTI-C12, our results show that upon shortening the side chain of BTTI, the hole mobility, film-forming capability, and resultant device performance were remarkably improved, with the device conversion efficiencies of 19.69% for BTTI-C6, 18.89% for BTTI-C8, and 17.49% for BTTI-C12. Meanwhile, compared to those made with the routine doped Spiro-OMeTAD, devices based on our dopant-free HTMs exhibited significantly improved stability. This work paves the way to the development of effective dopant-free HTMs for high-performance PSCs.

Backbone Coplanarity Tuning of 1,4-Di(3-alkoxy-2-thienyl)-2,5-difluorophenylene-Based Wide Bandgap Polymers for Efficient Organic Solar Cells Processed from Nonhalogenated Solvent.

Halogenated solvents are prevailingly used in the fabrication of nonfullerene organic solar cells (NF-OSCs) at the current stage, imposing significant restraints on their practical applications. By copolymerizing phthalimide or thieno[3,4-c]pyrrole-4,6-dione (TPD) with 1,4-di(3-alkoxy-2-thienyl)-2,5-difluorophenylene (DOTFP), which features intramolecular noncovalent interactions, the backbone planarity of the resulting DOTFP-based polymers can be effectively tuned, yielding distinct solubilities, aggregation characters, and chain packing properties. Polymer DOTFP-PhI with a more twisted backbone showed a lower degree of aggregation in solution but an increased film crystallinity than polymer DOTFP-TPD. An organic thin-film transistor and NF-OSC based on DOTFP-PhI, processed with a nonhalogenated solvent, exhibited a high hole mobility up to 1.20 cm2 V-1 s-1 and a promising power conversion efficiency up to 10.65%, respectively. The results demonstrate that DOTFP is a promising building block for constructing wide bandgap polymers and backbone coplanarity tuning is an effective strategy to develop high-performance organic semiconductors processable with a nonhalogenated solvent.

Dopant-Free Small-Molecule Hole-Transporting Material for Inverted Perovskite Solar Cells with Efficiency Exceeding 21.

Hole-transporting materials (HTMs) play a critical role in realizing efficient and stable perovskite solar cells (PVSCs). Considering their capability of enabling PVSCs with good device reproducibility and long-term stability, high-performance dopant-free small-molecule HTMs (SM-HTMs) are greatly desired. However, such dopant-free SM-HTMs are highly elusive, limiting the current record efficiencies of inverted PVSCs to around 19%. Here, two novel donor-acceptor-type SM-HTMs (MPA-BTI and MPA-BTTI) are devised, which synergistically integrate several design principles for high-performance HTMs, and exhibit comparable optoelectronic properties but distinct molecular configuration and film properties. Consequently, the dopant-free MPA-BTTI-based inverted PVSCs achieve a remarkable efficiency of 21.17% with negligible hysteresis and superior thermal stability and long-term stability under illumination, which breaks the long-time standing bottleneck in the development of dopant-free SM-HTMs for highly efficient inverted PVSCs. Such a breakthrough is attributed to the well-aligned energy levels, appropriate hole mobility, and most importantly, the excellent film morphology of the MPA-BTTI. The results underscore the effectiveness of the design tactics, providing a new avenue for developing high-performance dopant-free SM-HTMs in PVSCs.

Ruthenium acetylacetonate in interface engineering for high performance planar hybrid perovskite solar cells.

As it already made huge effect in the commercialization of silicon and other photovoltaics, interface engineering is dispensable in the current and future evolution of hybrid perovskite solar cells (PSCs) techniques. In order to solve carriers' recombination and detention at the cathode side of planar PSCs, in this work, Ruthenium acetylacetonate (RuAcac) was successfully adopted as a reliable and stable cathode interfacial layer (CIL) to improve the inverted planar PSCs. The power conversion efficiency of the optimal devices was enhanced from 12.74% for the control device without RuAcac, to 17.15% for the RuAcac based devices, with an open circuit voltage of 1.077 V, a short circuit current density of 21.28 mA/cm2, and fill factor of 74.7% correspondingly. A series of photon-physics and microscopy protocols, including EQE, UPS, XPS, PL and SKPM, were used to discover the function of RuAcac CIL. Those results confirms an identical conclusion that RuAcac enables the formation of quasi-ohmic contact at the cathode side by eliminating the energy level barrier between the LUMO of PCBM and Fermi level of silver electrode. The low temperature and facile processed Ruthenium acetylacetonate in this work definitely offer us a robust interface-engineering way for the perovskite solar cells and also their commercialization.

Metal Acetylacetonate Series in Interface Engineering for Full Low-Temperature-Processed, High-Performance, and Stable Planar Perovskite Solar Cells with Conversion Efficiency over 16% on 1 cm2 Scale.

A series of metal acetylacetonates produced by a full low-temperature (below 100 °C) process are successfully employed to obtain both "multistable" and high-performance planar-inverted perovskite solar cells. All the three kinds of champion cells in small area exhibit over 18% in conversion-efficiency with negligible hysteresis, along with a conversion efficiency above 16% for planar PSCs in an aperture area of over 1 cm2 .

Black Phosphorus Quantum Dots for Hole Extraction of Typical Planar Hybrid Perovskite Solar Cells.

Black phosphorus, famous as two-dimensional (2D) materials, shows such excellent properties for optoelectronic devices such as tunable direct band gap, extremely high hole mobility (300-1000 cm2/(V s)), and so forth. In this Letter, facile processed black phosphorus quantum dots (BPQDs) were successfully applied to enhance hole extraction at the anode side of the typical p-i-n planar hybrid perovskite solar cells, which remarkably improved the performance of devices with photon conversion efficiency ramping up from 14.10 to 16.69%. Moreover, more detailed investigations by c-AFM, SKPM, SEM, hole-only devices, and photon physics measurements discover further the hole extraction effect and work mechanism of the BPQDs, such as nucleation assistance for the growth of large grain size perovskite crystals, fast hole extraction, more efficient hole transfer, and suppression of energy-loss recombination at the anode interface. This work definitely paves the way for discovering more and more 2D materials with high electronic properties to be used in photovoltaics and optoelectronics.