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  1. Mohd Yusoff AR, Mat Teridi MA, Jang J
    Nanoscale, 2016 Mar 17;8(12):6328-34.
    PMID: 26489053 DOI: 10.1039/c5nr06234a
    Solution processed zirconium acetylacetonate (Zr(acac)) is successfully employed as an electron extraction layer, replacing conventional titanium oxide, in planar CH3NH3PbI3 perovskite solar cells. The as-prepared Zr(acac) film possesses high transparency, high conductivity, a smooth morphology, high wettability, compatibility with PbI2 DMF solution, and an energy level matching that of CH3NH3PbI3 perovskite material. An average power conversion efficiency of about 11.93%, along with a high fill factor of 74.36%, an open circuit voltage of 1.03 V, and a short-circuit current density of 15.58 mA cm(-2) is achieved. The overall performance of the devices is slight better than that of cells using ruthenium acetylacetonate (Ru(acac)). The differences between solar cells with different electron extraction layers in charge recombination, charge transport and transfer and lifetime are further explored and it is demonstrate that Zr(acac) is a more effective and promising electron extraction layer. This work provides a simple, and cost effective route for the preparation of an effective hole extraction layer.
  2. Teridi MA, Sookhakian M, Basirun WJ, Zakaria R, Schneider FK, da Silva WJ, et al.
    Nanoscale, 2015 Apr 28;7(16):7091-100.
    PMID: 25640454 DOI: 10.1039/c4nr05874g
    High performance organic devices including polymer solar cells (PSCs) and light emitting diodes (PLEDs) were successfully demonstrated with the presence of highly ordered nanoimprinted Au nanodisks (Au NDs) in their solution-processed active/emissive layers, respectively. PSCs and PLEDs were fabricated using a low bandgap polymer and acceptor, nitrogen doped multiwalled carbon nanotubes poly[4,8-bis[(2-ethylhexyl)oxy]benzo[1,2-b:4,5-b']dithiophene-2,6-diyl][3-fluoro-2-[(2-ethylhexyl)carbonyl] thieno[3,4-b]-thiophenediyl] (n-MWCNTs:PTB7), and [6,6]-phenyl C71 butyric acid methyl ester (PC71BM) and (4,4-N,N-dicarbazole) biphenyl (CBP) doped with tris(2-phenylpyridine) iridium(iii) (Ir(ppy)3) as active/emissive layers, respectively. We synthesized nitrogen doped graphene and used it as anodic buffer layer in both devices. The localized surface plasmon resonance (LSPR) effect from Au NDs clearly contributed to the increase in light absorption/emission in the active layers from electromagnetic field enhancement, which originated from the excited LSPR in PSCs and PLEDs. In addition to the high density of LSPR and strong exciton-SP coupling, the electroluminescent (EL) enhancement is ascribed to enhanced spontaneous emission rates. This is due to the plasmonic near-field effect induced by Au NDs. The PSCs and PLEDs exhibited 14.98% (8.08% to 9.29%) under one sun of simulated air mass 1.5 global (AM1.5G) illumination (100 mW cm(-2)) and 19.18% (8.24 to 9.82 lm W(-1)) enhancement in the power conversion efficiencies (PCEs) compared to the control devices without Au NDs.
  3. Toh PY, Ng BW, Ahmad AL, Chieh DC, Lim J
    Nanoscale, 2014 Nov 7;6(21):12838-48.
    PMID: 25227473 DOI: 10.1039/c4nr03121k
    Successful application of a magnetophoretic separation technique for harvesting biological cells often relies on the need to tag the cells with magnetic nanoparticles. This study investigates the underlying principle behind the attachment of iron oxide nanoparticles (IONPs) onto microalgal cells, Chlorella sp. and Nannochloropsis sp., in both freshwater and seawater, by taking into account the contributions of various colloidal forces involved. The complex interplay between van der Waals (vdW), electrostatic (ES) and Lewis acid-base interactions (AB) in dictating IONP attachment was studied under the framework of extended Derjaguin-Landau-Verwey-Overbeek (XDLVO) analysis. Our results showed that ES interaction plays an important role in determining the net interaction between the Chlorella sp. cells and IONPs in freshwater, while the AB and vdW interactions play a more dominant role in dictating the net particle-to-cell interaction in high ionic strength media (≥100 mM NaCl), such as seawater. XDLVO predicted effective attachment between cells and surface functionalized IONPs (SF-IONPs) with an estimated secondary minimum of -3.12 kT in freshwater. This prediction is in accordance with the experimental observation in which 98.89% of cells can be magnetophoretically separated from freshwater with SF-IONPs. We have observed successful magnetophoretic separation of microalgal cells from freshwater and/or seawater for all the cases as long as XDLVO analysis predicts particle attachment. For both the conditions, no pH adjustment is required for particle-to-cell attachment.
  4. Arora VK, Bhattacharyya A
    Nanoscale, 2013 Nov 21;5(22):10927-35.
    PMID: 24061093 DOI: 10.1039/c3nr03814a
    An integrated cohesive band structure of carbon nanotubes (CNTs) applicable to all chirality directions (n, m), starting from the Dirac cone of a graphene nanolayer in k-space, is demarcated, in direct contrast to dissimilar chiral and achiral versions in the published literature. The electron wave state of a CNT is quantized into one-dimensional (1-D) nanostructure with a wrapping mode, satisfying the boundary conditions from one Dirac K-point to an equivalent neighboring one with an identical phase and returning to the same K point. The repetitive rotation for an identical configuration with added band index (n-m)mod3, yields one metallic (M) with zero bandgap corresponding to (n-m)mod3 = 0, semiconducting state SC1 with (n-m)mod3 = 1 and SC2 with (n-m)mod3 = 2. The band gap and effective mass of SC2 state are twice as large as those of SC1 state. A broad-spectrum expression signifying the linear dependence of the effective mass on the bandgap is obtained. Both the Fermi energy and the intrinsic velocity limiting the current to the saturation level is calculated as a function of the carrier concentration. Limitations of the parabolic approximation are pointed out. Several new features of the band structure are acquired in a seamlessly unified mode for all CNTs, making it suitable for all-encompassing applications. Applications of the theory to high-field transport are advocated with an example of a metallic CNT, in agreement with experimental observations. The mechanism behind the breakdown of the linear current-voltage relation of Ohm's law and the associated surge in resistance are explained on the basis of the nonequilibrium Arora's distribution function (NEADF). These results are important for the performance evaluation and characterization of a variety of applications on CNT in modern nanoscale circuits and devices.
  5. Shi X, Wu X, Song T, Li X
    Nanoscale, 2016 Jul 22.
    PMID: 27444699
    The design of DNA nanotubes is a promising and hot research branch in structural DNA nanotechnology, which is rapidly developing as a versatile method for achieving subtle nanometer scale materials and molecular diagnostic/curative devices. Multifarious methods have been proposed to achieve varied DNA nanotubes, such as using square tiles and single-stranded tiles, but it is still a challenge to develop a bottom-up assembly way to build DNA nanotubes with different diameters and patterns using certain universal DNA nanostructures. This work addresses the challenge by assembling three types of spatial DNA nanotubes with different diameters and patterns from the so-called "basic bricks", i.e., hierarchical DNA sub-tiles. A high processing rate and throughput synthesis of DNA nanotubes are observed and analyzed by atomic force microscopy. Experimental observations and data analysis suggests the stability and controllability of DNA nanotubes assembled by hierarchical DNA sub-tiles.
  6. New SY, Lee ST, Su XD
    Nanoscale, 2016 Oct 20;8(41):17729-17746.
    PMID: 27722695
    12 years after the introduction of DNA-templated silver nanoclusters (DNA-AgNCs), exciting progress has been made and yet we are still in the midst of trying to fully understand this nanomaterial. The prominent excellence of DNA-AgNCs is undoubtedly its modulatable emission property, of which how variation in DNA templates causes emission tuning remains elusive. Based on the up-to-date DNA-AgNCs, we aim to establish the correlation between the structure/sequence of DNA templates and emission behaviour of AgNCs. Herein, we systematically present a wide-range of DNA-AgNCs based on the structural complexity of the DNA templates, including single-stranded DNA (ssDNA), double-stranded DNA (dsDNA), triple-stranded DNA (tsDNA) and DNA nanostructures. For each DNA category, we discuss the emission property, quantum yield and synthesis condition of the respective AgNCs, before cross-comparing the impact of different DNA scaffolds on the properties of AgNCs. A future outlook for this area is given as a conclusion. By putting the information together, this review may shed new light on understanding DNA-AgNCs while we are expecting continuous breakthroughs in this field.
  7. Huang YL, Chang WS, Van CN, Liu HJ, Tsai KA, Chen JW, et al.
    Nanoscale, 2016 Aug 25;8(34):15795-801.
    PMID: 27533610 DOI: 10.1039/c6nr04997d
    Ferroelectric photoelectrodes, other than conventional semiconductors, are alternative photo-absorbers in the process of water splitting. However, the capture of photons and efficient transfer of photo-excited carriers remain as two critical issues in ferroelectric photoelectrodes. In this work, we overcome the aforementioned issues by decorating the ferroelectric BiFeO3 (BFO) surface with Au nanocrystals, and thus improving the photoelectrochemical (PEC) performance of BFO film. We demonstrate that the internal field induced by the spontaneous polarization of BFO can (1) tune the efficiency of the photo-excited carriers' separation and charge transfer characteristics in bare BFO photoelectrodes, and (2) modulate an extra optical absorption within the visible light region, created by the surface plasmon resonance excitation of Au nanocrystals to capture more photons in the Au/BFO heterostructure. This study provides key insights for understanding the tunable features of PEC performance, composed of the heterostructure of noble metals and ferroelectric materials.
  8. Trache D, Hussin MH, Haafiz MK, Thakur VK
    Nanoscale, 2017 Feb 02;9(5):1763-1786.
    PMID: 28116390 DOI: 10.1039/c6nr09494e
    Cellulose nanocrystals, a class of fascinating bio-based nanoscale materials, have received a tremendous amount of interest both in industry and academia owing to its unique structural features and impressive physicochemical properties such as biocompatibility, biodegradability, renewability, low density, adaptable surface chemistry, optical transparency, and improved mechanical properties. This nanomaterial is a promising candidate for applications in fields such as biomedical, pharmaceuticals, electronics, barrier films, nanocomposites, membranes, supercapacitors, etc. New resources, new extraction procedures, and new treatments are currently under development to satisfy the increasing demand of manufacturing new types of cellulose nanocrystals-based materials on an industrial scale. Therefore, this review addresses the recent progress in the production methodologies of cellulose nanocrystals, covering principal cellulose resources and the main processes used for its isolation. A critical and analytical examination of the shortcomings of various approaches employed so far is made. Additionally, structural organization of cellulose and nomenclature of cellulose nanomaterials have also been discussed for beginners in this field.
  9. Fonseka HA, Ameruddin AS, Caroff P, Tedeschi D, De Luca M, Mura F, et al.
    Nanoscale, 2017 Sep 21;9(36):13554-13562.
    PMID: 28872181 DOI: 10.1039/c7nr04598k
    The usability and tunability of the essential InP-InGaAs material combination in nanowire-based quantum wells (QWs) are assessed. The wurtzite phase core-multi-shell InP-InGaAs-InP nanowire QWs are characterised using cross-section transmission electron microscopy and photoluminescence measurements. The InP-InGaAs direct interface is found to be sharp while the InGaAs-InP inverted interface is more diffused, in agreement with their planar counterpart. Bright emission is observed from the single nanowires containing the QWs at room temperature, with no emission from the InP core or outer barrier. The tunability of the QW emission wavelength in the 1.3-1.55 μm communication wavelength range is demonstrated by varying the QW thickness and in the 1.3 μm range by varying the composition. The experiments are supported by simulation of the emission wavelength of the wurtzite phase InP-InGaAs QWs in the thickness range considered. The radial heterostructure is further extended to design multiple QWs with bright emission, therefore establishing the capability of this material system for nanowire based optical devices for communication applications.
  10. Ong WJ, Tan LL, Chai SP, Yong ST, Mohamed AR
    Nanoscale, 2014 Feb 21;6(4):1946-2008.
    PMID: 24384624 DOI: 10.1039/c3nr04655a
    Titanium dioxide (TiO2) is one of the most widely investigated metal oxides due to its extraordinary surface, electronic and catalytic properties. However, the large band gap of TiO2 and massive recombination of photogenerated electron-hole pairs limit its photocatalytic and photovoltaic efficiency. Therefore, increasing research attention is now being directed towards engineering the surface structure of TiO2 at the most fundamental and atomic level namely morphological control of {001} facets in the range of microscale and nanoscale to fine-tune its physicochemical properties, which could ultimately lead to the optimization of its selectivity and reactivity. The synthesis of {001}-faceted TiO2 is currently one of the most active interdisciplinary research areas and demonstrations of catalytic enhancement are abundant. Modifications such as metal and non-metal doping have also been extensively studied to extend its band gap to the visible light region. This steady progress has demonstrated that TiO2-based composites with {001} facets are playing and will continue to play an indispensable role in the environmental remediation and in the search for clean and renewable energy technologies. This review encompasses the state-of-the-art research activities and latest advancements in the design of highly reactive {001} facet-dominated TiO2via various strategies, including hydrothermal/solvothermal, high temperature gas phase reactions and non-hydrolytic alcoholysis methods. The stabilization of {001} facets using fluorine-containing species and fluorine-free capping agents is also critically discussed in this review. To overcome the large band gap of TiO2 and rapid recombination of photogenerated charge carriers, modifications are carried out to manipulate its electronic band structure, including transition metal doping, noble metal doping, non-metal doping and incorporating graphene as a two-dimensional (2D) catalyst support. The advancements made in these aspects are thoroughly examined, with additional insights related to the charge transfer events for each strategy of the modified-TiO2 composites. Finally, we offer a summary and some invigorating perspectives on the major challenges and new research directions for future exploitation in this emerging frontier, which we hope will advance us to rationally harness the outstanding structural and electronic properties of {001} facets for various environmental and energy-related applications.
  11. Ang KM, Yeo LY, Hung YM, Tan MK
    Nanoscale, 2017 May 18;9(19):6497-6508.
    PMID: 28466906 DOI: 10.1039/c7nr01690e
    We exploit the possibility of enhancing the molecular transport of liquids through graphene films using amplitude modulated surface acoustic waves (SAWs) to demonstrate effective and efficient nanoparticle filtration. The use of the SAW, which is an extremely efficient means for driving microfluidic transport, overcomes the need for the large mechanical pumps required to circumvent the large pressure drops encountered in conventional membranes for nanoparticle filtration. 100% filtration efficiency was obtained for micron-dimension particulates, decreasing to only 95% for the filtration of particles of tens of nanometers in dimension, which is comparable to that achieved with other methods. To circumvent clogging of the film, which is typical with all membrane filters, a backwash operation to flush the nanoparticles is incorporated simply by reversing the SAW-induced flow such that 98% recovery of the initial filtration rate is recovered. Given these efficiencies, together with the low cost and compact size of the chipscale SAW devices, we envisage the possibility of scaling out the process by operating a large number of devices in parallel to achieve typical industrial-scale throughputs with potential benefits in terms of substantially lower capital, operating and maintenance costs.
  12. Chu RX, Lin J, Wu CQ, Zheng J, Chen YL, Zhang J, et al.
    Nanoscale, 2017 Jun 23.
    PMID: 28644506 DOI: 10.1039/c7nr02423a
    Lithium-sulfur (Li-S) batteries have attracted great attention owing to their excellent electrochemical properties, such as the high discharge voltage of 2.3 V, specific capacity of 1675 mA h g(-1) and energy density of 2600 Wh kg(-1). The widely used slurry made electrodes of Li-S batteries are plagued by the serious shuttle effect and insulating nature of sulfur. Herein, a reduced graphene oxide coated porous carbon nanofiber flexible paper (rGO@S-PCNP) was fabricated and directly used as an additive-free cathode for Li-S batteries. The results show that the rGO@S-PCNP is certified to be effective at relieving the shuttle effect and improving the conductivity, thus achieving high electrochemical performance. The rGO@S-PCNP composite with a sulfur content of 58.4 wt% delivers a high discharge capacity of 623.7 mA h g(-1) after 200 cycles at 0.1 C (1 C = 1675 mA g(-1)) with the average Coulombic efficiency of 97.1%. The excellent cyclability and high Coulombic efficiency indicate that the as-prepared rGO@S-PCNP composite paper can be a promising cathode for lithium-sulfur batteries, and is envisioned to have great potential in high energy density flexible power devices. This facile strategy brings great significance for large-scale industrial fabrication of flexible lithium-sulfur batteries.
  13. Iwasaki T, Muruganathan M, Schmidt ME, Mizuta H
    Nanoscale, 2017 Jan 26;9(4):1662-1669.
    PMID: 28074959 DOI: 10.1039/c6nr08117g
    The transformation of systematic vacuum and hydrogen annealing effects in graphene devices on the SiO2 surface is reported based on experimental and van der Waals interaction corrected density functional theory (DFT) simulation results. Vacuum annealing removes p-type dopants and reduces charged impurity scattering in graphene. Moreover, it induces n-type doping into graphene, leading to the improvement of the electron mobility and conductivity in the electron transport regime, which are reversed by exposing to atmospheric environment. On the other hand, annealing in hydrogen/argon gas results in smaller n-type doping along with a decrease in the overall conductivity and carrier mobility. This degradation of the conductivity is irreversible even the graphene devices are exposed to ambience. This was clarified by DFT simulations: initially, silicon dangling bonds were partially terminated by hydrogen, subsequently, the remaining dangling bonds became active and the distance between the graphene and SiO2 surface decreased. Moreover, both annealing methods affect the graphene channel including the vicinity of the metal contacts, which plays an important role in asymmetric carrier transport.
  14. Kuche K, Maheshwari R, Tambe V, Mak KK, Jogi H, Raval N, et al.
    Nanoscale, 2018 May 17;10(19):8911-8937.
    PMID: 29722421 DOI: 10.1039/c8nr01383g
    The search for effective and non-invasive delivery modules to transport therapeutic molecules across skin has led to the discovery of a number of nanocarriers (viz.: liposomes, ethosomes, dendrimers, etc.) in the last few decades. However, available literature suggests that these delivery modules face several issues including poor stability, low encapsulation efficiency, and scale-up hurdles. Recently, carbon nanotubes (CNTs) emerged as a versatile tool to deliver therapeutics across skin. Superior stability, high loading capacity, well-developed synthesis protocol as well as ease of scale-up are some of the reason for growing interest in CNTs. CNTs have a unique physical architecture and a large surface area with unique surface chemistry that can be tailored for vivid biomedical applications. CNTs have been thus largely engaged in the development of transdermal systems such as tuneable hydrogels, programmable nonporous membranes, electroresponsive skin modalities, protein channel mimetic platforms, reverse iontophoresis, microneedles, and dermal buckypapers. In addition, CNTs were also employed in the development of RNA interference (RNAi) based therapeutics for correcting defective dermal genes. This review expounds the state-of-art synthesis methodologies, skin penetration mechanism, drug liberation profile, loading potential, characterization techniques, and transdermal applications along with a summary on patent/regulatory status and future scope of CNT based skin therapeutics.
  15. Etesami M, Abouzari-Lotf E, Sha'rani SS, Miyake M, Moozarm Nia P, Ripin A, et al.
    Nanoscale, 2018 Jul 13;10(27):13212-13222.
    PMID: 29971298 DOI: 10.1039/c8nr02450b
    A novel polyoxometalate-based electrode was developed by incorporating phosphotungstic acid (PWA) in nylon-6,6 nanofiber, followed by carbonization. The developed PWA-carbon nanofiber (PWA-CNF) showed the characteristics of the dual-scale porosity of micro- and mesoporous substrate with surface area of around 684 m2 g-1. The compound exhibited excellent stability in vanadium electrolyte and battery cycling. Evaluation of electrocatalytic properties toward V2+/V3+ and VO2+/VO2+ redox couples indicated promising advantages in electron transfer kinetics and increasing energy efficiency, particularly for the VO2+/VO2+ couple. Moreover, the developed electrode exhibited substantially improved energy efficiency (14% higher than that of pristine carbon felt) in the single cell vanadium redox flow battery. This outstanding performance was attributed to high surface area and abundant oxygen-containing linkages in the developed electrode.
  16. Chen Y, Ge D, Zhang J, Chu R, Zheng J, Wu C, et al.
    Nanoscale, 2018 Sep 20;10(36):17378-17387.
    PMID: 30203824 DOI: 10.1039/c8nr01195h
    Tin-based materials have been intensively studied as attractive candidates for high-capacity and long-cycle-life anodes in Li-ion batteries (LIBs) owing to their low cost and high energy density. However, they all suffer from severe structural decay during the lithium ion insertion/extraction process, which results in deterioration in the overall performance of the batteries. To mitigate this problem, we have synthesized a Mo-doped SnO2 nanostructure via a facile hydrothermal method, which then fragmented into ultrafine particles after dozens of cycles. The fracture-resistant size and ample contact with Super-P and Li2O greatly improved the electrochemical kinetics and cyclability to deliver a reversible capacity of 670 mA h g-1 after 700 cycles, which demonstrated the potential suitability of Mo-doped SnO2 nanoparticles as a long-cycle-life anode material. Then, the compounds were uniformly dispersed in carbon nanofibers and reduced in situ to prepare a free-standing anode via electrospinning and carbonization. When used directly as an anode in LIBs (without a polymeric binder or conductive agent, as well as a current collector), the nanofiber membrane anode delivered comparable cycling performance and capacity to that of a slurry-coated electrode.
  17. Nasaruddin RR, Yao Q, Chen T, Hülsey MJ, Yan N, Xie J
    Nanoscale, 2018 Dec 04.
    PMID: 30512030 DOI: 10.1039/c8nr07197g
    Quasi-homogeneous ligand-protected gold nanoclusters (Au NCs) with atomic precision and well-defined structure offer great opportunity for exploring the catalytic nature of nanogold catalysts at a molecular level. Herein, using real-time electrospray ionization mass spectrometry (ESI-MS), we have successfully identified the desorption and re-adsorption of p-mercaptobenzoic acid (p-MBA) ligands from Au25(p-MBA)18 NC catalysts during the hydrogenation of 4-nitrophenol in solution. This ligand dynamic (desorption and re-adsorption) would initiate structural transformation of Au25(p-MBA)18 NC catalysts during the reaction, forming a mixture of smaller Au NCs (Au23(p-MBA)16 as the major species) at the beginning of catalytic reaction, which could further be transformed into larger Au NCs (Au26(p-MBA)19 as the major species). The adsorption of hydrides (from NaBH4) is identified as the determining factor that could induce the ligand dynamic and structural transformation of NC catalysts. This study provides fundamental insights into the catalytic nature of Au NCs, including catalytic mechanism, active species and stability of Au NC catalysts during a catalytic reaction.
  18. Xu Q, Li W, Ding L, Yang W, Xiao H, Ong WJ
    Nanoscale, 2019 Jan 23;11(4):1475-1504.
    PMID: 30620019 DOI: 10.1039/c8nr08738e
    Metal-free carbonaceous nanomaterials have witnessed a renaissance of interest due to the surge in the realm of nanotechnology. Among myriads of carbon-based nanostructures with versatile dimensionality, one-dimensional (1D) carbon nanotubes (CNTs) and zero-dimensional (0D) carbon dots (CDs) have grown into a research frontier in the past few decades. With extraordinary mechanical, thermal, electrical and optical properties, CNTs are utilized in transparent displays, quantum wires, field emission transistors, aerospace materials, etc. Although CNTs possess diverse characteristics, their most attractive property is their unique photoluminescence. On the other hand, another growing family of carbonaceous nanomaterials, which is CDs, has drawn much research attention due to its cost-effectiveness, low toxicity, environmental friendliness, fluorescence, luminescence and simplicity to be synthesized and functionalized with surface passivation. Benefiting from these unprecedented properties, CDs have been widely employed in biosensing, bioimaging, nanomedicine, and catalysis. Herein, we have systematically presented the fascinating properties, preparation methods and multitudinous applications of CNTs and CDs (including graphene quantum dots). We will discuss how CNTs and CDs have emerged as auspicious nanomaterials for potential applications, especially in electronics, sensors, bioimaging, wearable devices, batteries, supercapacitors, catalysis and light-emitting diodes (LEDs). Last but not least, this review is concluded with a summary, outlook and invigorating perspectives for future research horizons in this emerging platform of carbonaceous nanomaterials.
  19. Brown AAM, Hooper TJN, Veldhuis SA, Chin XY, Bruno A, Vashishtha P, et al.
    Nanoscale, 2019 Jul 07;11(25):12370-12380.
    PMID: 31215940 DOI: 10.1039/c9nr02566a
    We report the self-assembly of an extensive inter-ligand hydrogen-bonding network of octylphosphonates on the surface of cesium lead bromide nanocrystals (CsPbBr3 NCs). The post-synthetic addition of octylphosphonic acid to oleic acid/oleylamine-capped CsPbBr3 NCs promoted the attachment of octylphosphonate to the NC surface, while the remaining oleylammonium ligands maintained the high dispersability of the NCs in non-polar solvent. Through powerful 2D solid-state 31P-1H NMR, we demonstrated that an ethyl acetate/acetonitrile purification regime was crucial for initiating the self-assembly of extensive octylphosphonate chains. Octylphosphonate ligands were found to preferentially bind in a monodentate mode through P-O-, leaving polar P[double bond, length as m-dash]O and P-OH groups free to form inter-ligand hydrogen bonds. The octylphosphonate ligand network strongly passivated the nanocrystal surface, yielding a fully-purified CsPbBr3 NC ink with PLQY of 62%, over 3 times higher than untreated NCs. We translated this to LED devices, achieving maximum external quantum efficiency and luminance of 7.74% and 1022 cd m-2 with OPA treatment, as opposed to 3.59% and 229 cd m-2 for untreated CsPbBr3 NCs. This represents one of the highest efficiency LEDs obtained for all-inorganic CsPbBr3 NCs, accomplished through simple, effective passivation and purification processes. The robust binding of octylphosphonates to the perovskite lattice, and specifically their ability to interlink through hydrogen bonding, offers a promising passivation approach which could potentially be beneficial across a breadth of halide perovskite optoelectronic applications.
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