Durable CO2 conversion in the proton-exchange membrane system.

Electrolysis that reduces carbon dioxide (CO2) to useful chemicals can, in principle, contribute to a more sustainable and carbon-neutral future1-6. However, it remains challenging to develop this into a robust process because efficient conversion typically requires alkaline conditions in which CO2 precipitates as carbonate, and this limits carbon utilization and the stability of the system7-12. Strategies such as physical washing, pulsed operation and the use of dipolar membranes can partially alleviate these problems but do not fully resolve them11,13-15. CO2 electrolysis in acid electrolyte, where carbonate does not form, has therefore been explored as an ultimately more workable solution16-18. Herein we develop a proton-exchange membrane system that reduces CO2 to formic acid at a catalyst that is derived from waste lead-acid batteries and in which a lattice carbon activation mechanism contributes. When coupling CO2 reduction with hydrogen oxidation, formic acid is produced with over 93% Faradaic efficiency. The system is compatible with start-up/shut-down processes, achieves nearly 91% single-pass conversion efficiency for CO2 at a current density of 600 mA cm-2 and cell voltage of 2.2 V and is shown to operate continuously for more than 5,200 h. We expect that this exceptional performance, enabled by the use of a robust and efficient catalyst, stable three-phase interface and durable membrane, will help advance the development of carbon-neutral technologies.

Sequential *CO management via controlling in situ reconstruction for efficient industrial-current-density CO2-to-C2+ electroreduction.

Sequentially managing the coverage and dimerization of *CO on the Cu catalysts is desirable for industrial-current-density CO2 reduction (CO2R) to C2+, which required the multiscale design of the surface atom/architecture. However, the oriented design is colossally difficult and even no longer valid due to unpredictable reconstruction. Here, we leverage the synchronous leaching of ligand molecules to manipulate the seeding-growth process during CO2R reconstruction and construct Cu arrays with favorable (100) facets. The gradient diffusion in the reconstructed array guarantees a higher *CO coverage, which can continuously supply the reactant to match its high-rate consumption for high partial current density for C2+. Sequentially, the lower energy barriers of *CO dimerization on the (100) facets contribute to the high selectivity of C2+. Profiting from this sequential *CO management, the reconstructed Cu array delivers an industrial-relevant FEC2+ of 86.1% and an FEC2H4 of 60.8% at 700 mA cm-2. Profoundly, the atomic-molecular scale delineation for the evolution of catalysts and reaction intermediates during CO2R can undoubtedly facilitate various electrocatalytic reactions.

Interlayer Delocalized Electrons Activate Basal Plane for Ultrahigh-Current-Density Hydrogen Evolution.

The basal plane of transition metal dichalcogenides (TMDCs) is inert for the hydrogen evolution reaction (HER) due to its low-efficiency charge transfer kinetics. We propose a strategy of filling the van der Waals (vdW) layer with delocalized electrons to enable vertical penetration of electrons from the collector to the adsorption intermediate vertically. Guided by density functional theory, we achieve this concept by incorporating Cu atoms into the interlayers of tantalum disulfide (TaS2). The delocalized electrons of d-orbitals of the interlayered Cu can constitute the charge transfer pathways in the vertical direction, thus overcoming the hopping migration through vdW gaps. The vertical conductivity of TaS2 increased by 2 orders of magnitude. The TaS2 basal plane HER activity was extracted with an on-chip microcell. Modified by the delocalized electrons, the current density increased by 20 times, reaching an ultrahigh value of 800 mA cm-2 at -0.4 V without iR compensation.

General phase-difference imaging of incoherent digital holography.

The hologram formed by incoherent holography based on self-interference should preserve the phase difference information of the object, such as the phase difference between the mutually orthogonal polarizations of anisotropic object. How to decode this phase difference from this incoherent hologram, i.e., phase-difference imaging, is of great significance for studying the properties of the measured object. However, there is no general phase-difference imaging theory due to both diverse incoherent holography systems and the complicated reconstruction process from holograms based on the diffraction theory. To realize phase-difference image in incoherent holography, the relationship between the phase difference of the object and the image reconstructed by holograms is derived using a general physical model of incoherent holographic systems, and then the additional phase that will distort this relationship in actual holographic systems is analyzed and eliminated. Finally, the phase-difference imaging that is suitable for the most incoherent holographic systems is realized and the general theory is experimentally verified. This technology can be applied to phase-difference imaging of anisotropic objects, and has potential applications in materials science, biomedicine, polarized optics and other fields.

Frequency selection rule for the HDHF Lissajous scanning imaging with a low-voltage one axis actuated PZT scanner based on an asymmetric fiber cantilever.

Lissajous micro scanners are very attractive in compact laser scanning applications for biomedical endoscopic imaging, such as confocal microscopy, endomicroscopy or optical coherence tomography. The scanning frequencies have a very important effect on the quality of the resulting Lissajous scanning imaging. In this paper, we propose a frequency selection rule for high definition and high frame-rate (HDHF) Lissajous scanning imaging, by deriving the relationship among the scanning field of view (FOV), actuation frequencies and pixel size based on the characteristics of the scanning trajectory. The minimum sampling rate based on the proposed frequency selection rule is further discussed. We report a lead zirconate titanate piezoelectric ceramic (PZT) based Lissajous fiber scanner to achieve HDHF Lissajous scanning imaging. Based on the frequency selection rule, different frequency combinations are calculated, under which the Lissajous fiber scanner can work at the frame rate (FR) of 10 Hz, 20 Hz, 40 Hz and 52 Hz. The trajectory evolution of the Lissajous scanning at the frame rate of 10 Hz has been obtained to verify the applicability of the proposed rule. The measured resolution of the scanner is 50.8 lp/mm at the unit optical magnification, and the measured FOV at the FR of 10 Hz and 40 Hz are 1.620 mm ×1.095 mm and 0.405 mm ×0.27 mm, respectively. HDHF Lissajous scanning images of the customized spatial varying binary pattern are obtained and reconstructed at the FR of 10 Hz and 40 Hz, demonstrating the practicability of the frequency selection rule.

Full-range depth-encoded swept source polarization sensitive optical coherence tomography.

To realize the high sensitivity polarization sensitive optical coherence tomography (PS-OCT) imaging, a fiber-based full-range depth-encoded swept source PS-OCT (SS-PS-OCT) method is proposed. The two OCT images corresponding to the orthogonal polarized input light are located on the high sensitivity imaging region of the opposite sides relative to the zero optical path difference position. The full-range OCT images can be obtained by implementing the spatial phase modulation in the reference arm. The detection sensitivity of the system was measured experimentally to be 67 dB when the imaging depth approaching to 2 mm. The imaging of the biological tissue verifies that the proposed full-range depth-encoded SS-PS-OCT system has the higher detection sensitivity compared with the conventional depth encoded SS-PS-OCT system. Finally, we demonstrated the full-range high sensitivity phase retardation image of the bovine tendon and skin of human fingertip. The fiber-based full-range depth-encoded SS-PS-OCT method can realize the high sensitivity birefringence imaging in the medical diagnosis scenes with the requirements for long imaging range and high detection sensitivity.

Imaging objects hidden inside the strongly scattering media based on bidirectional ghost imaging.

We demonstrate a novel, to the best of our knowledge, method for imaging objects hidden inside the strongly scattering media based on bidirectional ghost imaging (GI). In this method, GI is performed separately on both sides of the object, resulting in two GI results. Through an autocorrelation operation to the two GI results, the convolution between the autocorrelation of the object and the point spread function (PSF) of the strongly scattering media can be recovered. Therefore, the object can be recovered by obtaining the PSF of the strongly scattering media through noninvasive measurement or numerical calculation. Simulation and experimental results show that bidirectional ghost imaging (BGI) can reconstruct high-quality images, particularly when the thickness of the strongly scattering media greatly exceeds the scattering mean free path.

Imaging through thick scattering media based on envelope-informed learning with a simulated training dataset.

Computational imaging faces significant challenges in dealing with multiple scattering through thick complex media. While deep learning has addressed some ill-posed problems in scattering imaging, its practical application is limited by the acquisition of the training dataset. In this study, the Gaussian-distributed envelope of the speckle image is employed to simulate the point spread function (PSF), and the training dataset is obtained by the convolution of the handwritten digits with the PSF. This approach reduces the requirement of time and conditions for constructing the training dataset and enables a neural network trained on this dataset to reconstruct objects obscured by an unknown scattering medium in real experiments. The quality of reconstructed objects is negatively correlated with the thickness of the scattering medium. Our proposed method provides a new way, to the best of our knowledge, to apply deep learning in scattering imaging by reducing the time needed for constructing the training dataset.

Reconstructing Hydrogen-Bond Network for Efficient Acidic Oxygen Evolution.

Developing highly active oxygen evolution reaction (OER) catalysts in acidic conditions is a pressing demand for proton-exchange membrane water electrolysis. Manipulating proton character at the electrified interface, as the crux of all proton-coupled electrochemical reactions, is highly desirable but elusive. Herein we present a promising protocol, which reconstructs a connected hydrogen-bond network between the catalyst-electrolyte interface by coupling hydrophilic units to boost acidic OER activity. Modelling on N-doped-carbon-layer clothed Mn-doped-Co3O4 (Mn-Co3O4@CN), we unravel that the hydrogen-bond interaction between CN units and H2O molecule not only drags the free water to enrich the surface of Mn-Co3O4 but also serves as a channel to promote the dehydrogenation process. Meanwhile, the modulated local charge of the Co sites from CN units/Mn dopant lowers the OER barrier. Therefore, Mn-Co3O4@CN surpasses RuO2 at high current density (100 mA cm-2 @ ~538 mV).

Largely Pseudocapacitive Two-Dimensional Conjugated Metal-Organic Framework Anodes with Lowest Unoccupied Molecular Orbital Localized in Nickel-bis(dithiolene) Linkages.

Although two-dimensional conjugated metal-organic frameworks (2D c-MOFs) provide an ideal platform for precise tailoring of capacitive electrode materials, high-capacitance 2D c-MOFs for non-aqueous supercapacitors remain to be further explored. Herein, we report a novel phthalocyanine-based nickel-bis(dithiolene) (NiS4)-linked 2D c-MOF (denoted as Ni2[CuPcS8]) with outstanding pseudocapacitive properties in 1 M TEABF4/acetonitrile. Each NiS4 linkage is disclosed to reversibly accommodate two electrons, conferring the Ni2[CuPcS8] electrode a two-step Faradic reaction with a record-high specific capacitance among the reported 2D c-MOFs in non-aqueous electrolytes (312 F g-1) and remarkable cycling stability (93.5% after 10,000 cycles). Multiple analyses unveil that the unique electron-storage capability of Ni2[CuPcS8] originates from its localized lowest unoccupied molecular orbital (LUMO) over the nickel-bis(dithiolene) linkage, which allows the efficient delocalization of the injected electrons throughout the conjugated linkage units without inducing apparent bonding stress. The Ni2[CuPcS8] anode is used to demonstrate an asymmetric supercapacitor device that delivers a high operating voltage of 2.3 V, a maximum energy density of 57.4 Wh kg-1, and ultralong stability over 5000 cycles.

Tunable dual quasi-bound states in continuum and electromagnetically induced transparency enabled by the broken material symmetry in all-dielectric compound gratings.

Dual quasi-bound states in continuum (quasi-BICs) enabled by the broken geometric symmetry offer an effective way to design high-quality photonic devices, yet challenged by tunable functionalities. Here we employ the material asymmetry originating from the tunable material property of phase-change materials to design quasi-BICs in all-dielectric compound gratings. We find the even and odd quasi-BICs are modulated by the geometric and material asymmetries, respectively, and this effect is ensured by two different types of structural symmetries in the compound structure. Particularly, tunable electromagnetically induced transparency (EIT) can be achieved by modulating the material asymmetry. Furthermore, we systematically design the compound gratings consisting of the phase-change material of Sb2Se3 to demonstrate tunable dual quasi-BICs and EITs. Analytical calculations and numerical simulations are performed to verify these findings. Our work provides a promising way to enhance the flexibility of realizing quasi-BICs, which may boost tunable applications in nanodevices assisted by quasi-BICs.

Polarization-multiplexed, single-cavity dual-comb fiber laser based on a birefringent crystal and a saturable absorber.

We introduce a calcium carbonate birefringent crystal into an Er-fiber laser mode-locked by a saturable absorber, where dual-comb ultrashort pulses with orthogonal polarization have been obtained. The two ultrashort pulse trains from the laser exhibit polarization contrast ratios of 30 dB and 20 dB, indicating that the dual-comb mode-locking is due to the polarization-multiplexing mechanism. The dual-comb ultrashort pulses have central wavelengths of 1564.41 nm and 1564.51 nm, and pulse durations of 825 fs and 805 fs respectively. The optical spectra and pulse durations of the asynchronous ultrashort pulses are nearly identical, so that the output of the laser could be directly used for dual-comb applications. Besides, the repetition-rate difference of the two mode-locked pulses is 673 Hz, while its drift is only 0.093 Hz within 2 hours' time. The low drift of the repetition-rate difference manifests the single-cavity dual-comb Er-fiber laser has a high stability and high common-mode noise suppression. At last, we have tested the dual-comb fiber laser in a ranging experiment, where clear interferogram signal can be observed. The experimental results prove that this single-cavity dual-comb Er-fiber laser based on the birefringent crystal and saturable absorber can be a potential source for spectroscopy, optical imaging, absolute distance measurement and other dual-comb applications.

Controlling the directional excitation of surface plasmon polaritons using tunable non-Hermitian metasurfaces.

In this work, we propose an efficient approach to controlling the directional excitation of surface plasmon polaritons (SPPs) by dynamically modulating the real-part perturbation in a passive parity-time symmetric metasurface. This non-Hermitian system can experience two exceptional points that can induce two unidirectional excitation states of SPPs along opposite directions. Empowered by its superior modulation depth, the energy ratio and energy intensities of two excited SPP states can be effectively manipulated by this non-Hermitian metasurface. To demonstrate these findings, we design and numerically verify non-Hermitian metasurfaces integrated with an Sb2Se3 phase-change material. Our work provides a promising platform for the controllable engineering of SPP excitations, holding significant potential for the development of new plasmonic devices, including on-chip SPP sources, routers and sorters, and integrated optical circuits.

Switchable supermode emission in a doubly-coupled-ring system for multifunctional integrated photonic devices.

Effective integration of optical modes within chip-scale devices is critical to realize functional light emission, as it offers abundant physics and a versatile ability to control the mode evolution. Here, we present an efficient approach to achieve switchable emission by flexibly controlling supermode states in a doubly-coupled-ring system with four guided modes. The lasing conditions, which rely on the system's Hamiltonian, are revealed to yield multiple supermode states, including an exceptional-point state, a (quasi-)dark state, and a bright state. By freely engineering the coupling rate via phase-change material, the proposed system allows the generation of any desired states, enabling switchable and multifunctional emissions in fixed on-chip structures. Beyond the manipulation of various supermode emission states, our work presents a promising path toward the development of multifunctional integrated photonic devices, which may have applications in light storage, optical isolation, sensing, and so on.

Local polarization properties extraction using single incident state, single-mode-fiber-based spectral domain polarization-sensitive optical coherence tomography.

We showed the local polarization properties extraction method for the single incident state, all-single-mode-fiber-based spectral domain polarization-sensitive optical coherence tomography (SD-PS-OCT) system that uses the single linear-in-wavenumber spectral camera. Polarization controllers are used in the single-mode-fiber-based SD-PS-OCT system to provide a compact structure with polarization state stability. The local polarization properties of the birefringent sample are extracted from the cumulative polarization properties iteratively. The reconstructed polarization images demonstrate the local polarization properties extraction ability of the system.

miR-126 mitigates the osteogenic differentiation of human bone marrow-derived mesenchymal stem cells by targeting the ERK1/2 and Bcl-2 pathways.

Human bone marrow mesenchymal stem cells (hBMMSCs) are a promising cell source for bone engineering owing to their high potential to differentiate into osteoblasts. The objective of the present study is to assess microRNA-126 (miR-126) and examine its effects on the osteogenic differentiation of hBMMSCs. In this study, we investigate the role of miR-126 in the progression of osteogenic differentiation (OD) as well as the apoptosis and inflammation of hBMMSCs during OD induction. OD is induced in hBMMSCs, and matrix mineralization along with other OD-associated markers are evaluated by Alizarin Red S (AR) staining and quantitative PCR (qPCR). Gain- and loss-of-function studies are performed to demonstrate the role of miR-126 in the OD of hBMMSCs. Flow cytometry and qPCR-based cytokine expression studies are performed to investigate the effect of miR-126 on the apoptosis and inflammation of hBMMSCs. The results indicate that miR-126 expression is downregulated during the OD of hBMMSCs. Gain- and loss-of function assays reveal that miR-126 upregulation inhibits the differentiation of hBMMSCs into osteoblasts, whereas the downregulation of miR-126 promotes hBMMSC differentiation, as assessed by the determination of osteogenic genes and alkaline phosphatase activity. Furthermore, the miR-126 level is positively correlated with the production of inflammatory cytokines and apoptotic cell death. Additionally, our results suggest that miR-126 negatively regulates not only B-cell lymphoma 2 (Bcl-2) expression but also the phosphorylation of extracellular signal­regulated protein kinase (ERK) 1/2. Moreover, restoring ERK1/2 activity and upregulating Bcl-2 expression counteract the miR-126-mediated suppression of OD in hBMMSCs by promoting inflammation and apoptosis, respectively. Overall, our findings suggest a novel molecular mechanism relevant to the differentiation of hBMMSCs into osteoblasts, which can potentially facilitate bone formation by counteracting miR-126-mediated suppression of ERK1/2 activity and Bcl-2 expression.

On-Chip Microdevice Unveils Reactant Enrichment Effect Dominated Electrocatalysis Activity in Molecular-Linked Catalysts.

Molecular functionalization has been intensely studied and artificially constructed to advance various electrocatalytic processes. While there is a widely approved charge-doping effect, the underlying action for reactant distribution/transport remains long neglected. Here an on-chip microdevice unravels that the proton enrichment effect at prototypical methylene blue (MB)/MoS2 interfaces rather than charge doping contributes to the hydrogen evolution reaction (HER) activity. Back-gated electrical/electrochemical tests detect quantitatively a strong charge injection from MB to MoS2 realized over diploid carrier density, but these excess carriers are unqualified for the actual enhanced HER activity (from 32 to 125 mA cm-2 at -0.29 V). On-chip electrochemical impedance further certifies that the proton enrichment in the vicinity of MoS2, which is generated by the nucleophilic group of MB, actually dominates the HER activity. This finding uncovers the leading function of molecular-linked catalysts.

O-POSSUM and P-POSSUM as predictors of morbidity and mortality in older patients after hip fracture surgery: a meta-analysis.

BACKGROUND: The POSSUM model has been widely used to predict morbidity and mortality after general surgery. Modified versions known as O-POSSUM and P-POSSUM have been used extensively in orthopedic surgery, but their accuracy is unclear. This systematic review evaluated the predictive value of these models in older patients with hip fractures. METHODS: This study was performed and reported based on the "Preferred reporting items for systematic reviews and meta-analyses" guidelines. PubMed, Cochrane, EMBASE, and Web of Science were comprehensively searched for relevant studies, whose methodological quality was evaluated according to the "Methodological index for non-randomized studies" scale. Revman 5 was used to calculate weighted ratios of observed to expected morbidity or mortality. RESULTS: The meta-analysis included 10 studies, of which nine (2549 patients) assessed the ability of O-POSSUM to predict postoperative morbidity, nine (3649 patients) assessed the ability of O-POSSUM to predict postoperative mortality, and four (1794 patients) assessed the ability of P-POSSUM to predict postoperative mortality. The corresponding weighted ratios of observed to expected morbidity or mortality were 0.84 (95% CI 0.70-1.00), 0.68 (95% CI 0.49-0.95), and 0.61 (95% CI 0.16-2.38). CONCLUSIONS: While O-POSSUM shows reasonable accuracy in predicting postoperative morbidity in older patients with hip fractures, both P-POSSUM and O-POSSUM substantially overestimate postoperative mortality. The POSSUM model should be optimized further for this patient population.

Ultrahigh-Current-Density and Long-Term-Durability Electrocatalysts for Water Splitting.

Hydrogen economy is imagined where excess electric energy from renewable sources stored directly by electrochemical water splitting into hydrogen is later used as clean hydrogen fuel. Electrocatalysts with the superhigh current density (1000 mA cm-2 -level) and long-term durability (over 1000 h), especially at low overpotentials (<300 mV), seem extremely critical for green hydrogen from experiment to industrialization. Along the way, numerous innovative ideas are proposed to design high efficiency electrocatalysts in line with industrial requirements, which also stimulates the understanding of the mass/charge transfer and mechanical stability during the electrochemical process. It is of great necessity to summarize and sort out the accumulating knowledge in time for the development of laboratory to commercial use in this promising field. This review begins with examining the theoretical principles of achieving high-efficiency electrocatalysts with high current densities and excellent durability. Special attention is paid to acquaint efficient strategies to design perfect electrocatalysts including atomic structure regulation for electrical conductivity and reaction energy barrier, array configuration constructing for mass transfer process, and multiscale coupling for high mechanical strength. Finally, the importance and the personal perspective on future opportunities and challenges, is highlighted.