Integrative Analysis of Lactylome and Proteome of Hypertrophic Scar To Identify Pathways or Proteins Associated with Disease Development.

Lactylation (Kla), a recently discovered post-translational modification derived from lactate, plays crucial roles in various cellular processes. However, the specific influence of lactylation on the biological processes underlying hypertrophic scar formation remains unclear. In this study, we present a comprehensive profiling of the lactylome and proteome in both hypertrophic scars and adjacent normal skin tissues. A total of 1023 Kla sites originating from 338 nonhistone proteins were identified based on lactylome analysis. Proteome analysis in hypertrophic scar and adjacent skin samples revealed the identification of 2008 proteins. It is worth noting that Kla exhibits a preference for genes associated with ribosome function as well as glycolysis/gluconeogenesis in both normal skin and hypertrophic scar tissues. Furthermore, the functional enrichment analysis demonstrated that differentially lactyled proteins are primarily involved in proteoglycans, HIF-1, and AMPK signaling pathways. The combined analysis of the lactylome and proteome data highlighted a significant upregulation of 14 lactylation sites in hypertrophic scar tissues. Overall, our investigation unveiled the significant involvement of protein lactylation in the regulation of ribosome function as well as glycolysis/gluconeogenesis, potentially contributing to the formation of hypertrophic scars.

Sulfurization of bimetallic (Co and Fe) oxide and alloy decorated on multi-walled carbon nanotubes as efficient bifunctional electrocatalyst for water splitting.

The advancement in electrocatalysis, particularly in the development of efficient catalysts for hydrogen and oxygen evolution reactions (HER and OER), is crucial for sustainable energy generation through processes like overall water splitting. A notable bifunctional electrocatalyst, CoFe2O4/Co7Fe3, has been engineered to facilitate both OER and HER concurrently, aiming to reduce overpotentials. In the pursuit of further enhancing catalytic efficiency, a morphological transformation has been achieved by introducing a sulphur source and multi-walled carbon nanotubes (MWCNTs) into the catalyst system, resulting in S-CoFe2O4/Co7Fe3/MWCNTs. This modification has significantly improved the activity for both OER and HER. An onset overpotential of 250 mV@10 mAcm-2 for the OER and 270 mV@50 mAcm-2 for the HER, indicating efficient catalytic activity at relatively low overpotentials. S-CoFe2O4/Co7Fe3/MWCNTs display an outstanding long-term stability in alkaline electrolytes, with minimal Tafel slopes of 77 mV/dec for the OER and 70 mV/dec for the HER, suggesting sustained catalytic performance over extended periods. Furthermore, when employed as both the cathode and anode in the context of complete water splitting, S-CoFe2O4/Co7Fe3/MWCNTs demonstrate an impressive cell voltage of 1.52 V at a current density of 10 mA cm-2 in a 1 M KOH solution, showcasing its viability for practical applications. Given its cost-effectiveness and superior activity, S-CoFe2O4/Co7Fe3/MWCNTs hold significant promise for widespread applications in overall water splitting electrocatalysis, contributing to the advancement of cleaner and sustainable fuel generation technologies.

Boosting photo-thermal co-catalysis CO2 methanation by tuning interface electron transfer via Mott-Schottky heterojunction effect.

Photo-thermal co-catalytic reduction of CO2 to synthesize value-added chemicals presents a promising approach to addressing environmental issues. Nevertheless, traditional catalysts exhibit low light utilization efficiency, leading to the generation of a reduced number of electron-hole pairs and rapid recombination, thereby limiting catalytic performance enhancement. Herein, a Mott-Schottky heterojunction catalyst was developed by incorporating nitrogen-doped carbon coated TiO2 supported nickel (Ni) nanometallic particles (Ni/x-TiO2@NC). The optimal Ni/0.5-TiO2@NC sample displayed a conversion rate of 71.6 % and a methane (CH4) production rate of 65.3 mmol/(gcat·h) during photo-thermal co-catalytic CO2 methanation under full-spectrum illumination, with a CH4 selectivity exceeding 99.6 %. The catalyst demonstrates good stability as it shows no decay after two reaction cycles. The Mott-Schottky heterojunction catalysts display excellent efficiency in separating photo-generated electron-hole pairs and elevate the catalysts' temperature, thus accelerating the reaction rate. The in-situ experiments revealed that light-induced electron transfer effectively facilitates H2 dissociation and enhances surface defects, thereby promoting CO2 adsorption. This study introduces a novel approach for developing photo-thermal catalysts for CO2 reduction, aiming to enhance solar energy utilization and facilitate interface electron transfer.

Employing the Interpretable Ensemble Learning Approach to Predict the Bandgaps of the Halide Perovskites.

Halide perovskite materials have broad prospects for applications in various fields such as solar cells, LED devices, photodetectors, fluorescence labeling, bioimaging, and photocatalysis due to their bandgap characteristics. This study compiled experimental data from the published literature and utilized the excellent predictive capabilities, low overfitting risk, and strong robustness of ensemble learning models to analyze the bandgaps of halide perovskite compounds. The results demonstrate the effectiveness of ensemble learning decision tree models, especially the gradient boosting decision tree model, with a root mean square error of 0.090 eV, a mean absolute error of 0.053 eV, and a determination coefficient of 93.11%. Research on data related to ratios calculated through element molar quantity normalization indicates significant influences of ions at the X and B positions on the bandgap. Additionally, doping with iodine atoms can effectively reduce the intrinsic bandgap, while hybridization of the s and p orbitals of tin atoms can also decrease the bandgap. The accuracy of the model is validated by predicting the bandgap of the photovoltaic material MASn1-xPbxI3. In conclusion, this study emphasizes the positive impact of machine learning on material development, especially in predicting the bandgaps of halide perovskite compounds, where ensemble learning methods demonstrate significant advantages.

TiO2 Electron Transport Layer with p-n Homojunctions for Efficient and Stable Perovskite Solar Cells.

Low-temperature processed electron transport layer (ETL) of TiO2 that is widely used in planar perovskite solar cells (PSCs) has inherent low carrier mobility, resulting in insufficient photogenerated electron transport and thus recombination loss at buried interface. Herein, we demonstrate an effective strategy of laser embedding of p-n homojunctions in the TiO2 ETL to accelerate electron transport in PSCs, through localized build-in electric fields that enables boosted electron mobility by two orders of magnitude. Such embedding is found significantly helpful for not only the enhanced crystallization quality of TiO2 ETL, but the fabrication of perovskite films with larger-grain and the less-trap-states. The embedded p-n homojunction enables also the modulation of interfacial energy level between perovskite layers and ETLs, favoring for the reduced voltage deficit of PSCs. Benefiting from these merits, the formamidinium lead iodide (FAPbI3) PSCs employing such ETLs deliver a champion efficiency of 25.50%, along with much-improved device stability under harsh conditions, i.e., maintain over 95% of their initial efficiency after operation at maximum power point under continuous heat and illumination for 500 h, as well as mixed-cation PSCs with a champion efficiency of 22.02% and over 3000 h of ambient storage under humidity stability of 40%. Present study offers new possibilities of regulating charge transport layers via p-n homojunction embedding for high performance optoelectronics.

Highly Dispersed Mn-Doped Ceria Supported on N-Doped Carbon Nanotubes for Enhanced Oxygen Reduction Reaction.

The weak adsorption of oxygen on transition metal oxide catalysts limits the improvement of their electrocatalytic oxygen reduction reaction (ORR) performance. Herein, a dopamine-assisted method is developed to prepare Mn-doped ceria supported on nitrogen-doped carbon nanotubes (Mn-Ce-NCNTs). The morphology, dispersion of Mn-doped ceria, composition, and oxygen vacancies of the as-prepared catalysts were analyzed using various technologies. The results show that Mn-doped ceria was formed and highly dispersed on NCNTs, on which oxygen vacancies are abundant. The as-prepared Mn-Ce-NCNTs exhibit a high ORR performance, on which the average electron transfer number is 3.86 and the current density is 24.4% higher than that of commercial 20 wt % Pt/C. The peak power density of Mn-Ce-NCNTs is 68.1 mW cm-2 at the current density of 138.9 mA cm-2 for a Zn-air battery, which is close to that of 20 wt % Pt/C (69.4 mW cm-2 at 106.1 mA cm-2). Density functional theory (DFT) calculations show that the oxygen vacancy formation energies of Mn-doped CeO2(111) and pure CeO2(111) are -0.55 and 2.14 eV, respectively. Meanwhile, compared with undoped CeO2(111) (-0.02 eV), Mn-doped CeO2(111) easily adsorbs oxygen with the oxygen adsorption energy of only -0.68 eV. This work provides insights into the synergetic effect of Mn-doped ceria for facilitating oxygen adsorption and enhancing ORR performance.

Fe-Co heteronuclear atom pairs as catalytic sites for efficient oxygen electroreduction.

Single-site Fe-N-C catalysts are the most promising Pt-group catalyst alternatives for the oxygen reduction reaction, but their application is impeded by their relatively low activity and unsatisfactory stability as well as production costs. Here, cobalt atoms are introduced into an Fe-N-C catalyst to enhance its catalytic activity by utilizing the synergistic effect between Fe and Co atoms. Meanwhile, phenanthroline is employed as the ligand, which favours stable pyridinic N-coordinated Fe-Co sites. The obtained catalysts exhibit excellent ORR performance with a half-wave potential of 0.892 V and good stability under alkaline conditions. In addition, the excellent ORR activity and durability of FeCo-N-C enabled the constructed zinc-air battery to exhibit a high power density of 247.93 mW cm-2 and a high capacity of 768.59 mA h gZn-1. Moreover, the AEMFC based on FeCo-N-C also achieved a high open circuit voltage (0.95 V) and rated power density (444.7 mW cm-2), surpassing those of many currently reported transition metal-based cathodes. This work emphasizes the feasibility of this non-precious metal catalyst preparation strategy and its practical applicability in fuel cells and metal-air batteries.

Research progress of dual-atom site catalysts for photocatalysis.

Dual-atom site catalysts (DASCs) have sparked considerable interest in heterogeneous photocatalysis as they possess the advantages of excellent photoelectronic activity, photostability, and high carrier separation efficiency and mobility. The DASCs involved in these important photocatalytic processes, especially in the photocatalytic hydrogen evolution reaction (HER), CO2 reduction reaction (CO2RR), N2/nitrate reduction, etc., have been extensively investigated in the past few years. In this review, we highlight the recent progress in DASCs that provides fundamental insights into the photocatalytic conversion of small molecules. The controllable preparation and characterization methods of various DASCs are discussed. Subsequently, the reaction mechanisms of the formation of several important molecules (hydrogen, hydrocarbons and ammonia) on DASCs are introduced in detail, in order to probe the relationship between DASCs's structure and photocatalytic activity. Finally, some challenges and outlooks of DASCs in the photocatalytic conversion of small molecules are summarized and prospected. We hope that this review can provide guidance for in-depth understanding and aid in the design of efficient DASCs for photocatalysis.

Effects of oxygen vacancies and interfacial strain on the metal-insulator transition of VO2 nanobeams.

The role of oxygen vacancies and interfacial strain on the metal-insulator transition (MIT) behavior of high-quality VO2 nanobeams (NBs) synthesized on SiO2/Si substrates employing V2O5 as a precursor has been investigated in this research. Selective oxygen vacancies have been generated by argon plasma irradiation. The MIT is progressively suppressed as the duration of plasma processing increases; in addition, the temperature of MIT (TMIT) drops by up to 95 K relative to the pristine VO2 NBs. Incorporating oxygen vacancies into VO2 may increase its electron concentration, which might shift the Fermi levels upward, strengthen the electronic orbital overlap of the V-V chains, and further stabilize the metallic phase at lower temperatures, based on first-principles calculations. Furthermore, in order to evaluate the influence of substrate-induced strain in our situation, the MIT in two distinct types of VO2 NB samples is examined without metal contacts by using the distinctive light scattering characteristics of the metal (M) and insulator (I) phases (i.e., M/I domains) by optical microscopy. It is found that the domain structures in the "clamped" NBs persisted up to ∼453 K, while the "released" NBs (transferred to a new substrate) did not exhibit any domain structures and turned into an entirely M phase with a dark contrast above ∼348 K. When combined with first-principles calculations, the electronic orbital occupancy in the rutile phase contributes to explaining the interfacial strain-induced modulation of MIT. The current findings shed light on how interfacial strain and oxygen vacancies impact MIT behavior. It also suggests several types of control strategies for MIT in VO2 NBs, which are essential for a broader spectrum of VO2 NB applications.

Recent Progress of Transition Metal Selenides for Electrochemical Oxygen Reduction to Hydrogen Peroxide: From Catalyst Design to Electrolyzers Application.

Hydrogen peroxide (H2O2) is a highly value-added and environmental-friendly chemical with various applications. The production of H2O2 by electrocatalytic 2e- oxygen reduction reaction (ORR) has emerged as a promising alternative to the energy-intensive anthraquinone process. High selectivity Catalysts combining with superior activity are critical for the efficient electrosynthesis of H2O2. Earth-abundant transition metal selenides (TMSs) being discovered as a classic of stable, low-cost, highly active and selective catalysts for electrochemical 2e- ORR. These features come from the relatively large atomic radius of selenium element, the metal-like properties and the abundant reserves. Moreover, compared with the advanced noble metal or single-atom catalysts, the kinetic current density of TMSs for H2O2 generation is higher in acidic solution, which enable them to become suitable catalyst candidates. Herein, the recent progress of TMSs for ORR to H2O2 is systematically reviewed. The effects of TMSs electrocatalysts on the activity, selectivity and stability of ORR to H2O2 are summarized. It is intended to provide an insight from catalyst design and corresponding reaction mechanisms to the device setup, and to discuss the relationship between structure and activity.

Study on the vertical Bridgman method of melt-grown CsPbBr3 single crystals for nuclear radiation detection.

As an excellent representative of all-inorganic perovskite materials, CsPbBr3 has been widely used in high-energy rays or high-energy particles detection for its outstanding high carrier mobility and long diffusion length. The great challenges and opportunities in these fields are crystal growth technology, especially the high-quality and large-sized CsPbBr3 single crystals. In this work, the influences of growth parameters (temperature gradient, growth rate, cooling rate) and thermal stress by the vertical Bridgman method on the quality and performance of CsPbBr3 crystals are systematically studied. The final results show that 10°C cm-1 is the optimized temperature gradient and 0.5 mm h-1 is the suitable growth rate for CsPbBr3 crystal growth. The study also shows that a cooling rate of 10°C h-1 for the general temperature interval and 1°C h-1 for the phase transition temperature interval is helpful to balance crystal growth efficiency as well as crystal quality. Crystal cracks caused by thermal stress as well as crystal adhesion on the ampoule can be effectively solved by depositing a uniform carbon film on the ampoule in advance. The optical, electrical and detection performance are also investigated. The optical characterization in the wavelength region ranging from ultraviolet to infrared indicates the crystal has a low density of deep-level defects and good crystal quality. The resistivity over 109 Ω cm and µτ of electrons over 10-2 cm-2 V-1 proves that the electrical performance of the crystal has met the basic requirement for nuclear radiation detection. The metal-semiconductor-metal structure Ti/Ni/CsPbBr3/Ni/Ti detector fabricated from the optimized CsPbBr3 single crystal has an energy resolution of 12.85% (137Cs, 662 keV). The purpose of this work is to provide a useful guide and reference for the future exploration of repeatable and improvable CsPbBr3 crystal growth technology.

Advances in Heterogeneous Catalysts for Lignin Hydrogenolysis.

Lignin is the main component of lignocellulose and the largest source of aromatic substances on the earth. Biofuel and bio-chemicals derived from lignin can reduce the use of petroleum products. Current advances in lignin catalysis conversion have facilitated many of progress, but understanding the principles of catalyst design is critical to moving the field forward. In this review, the factors affecting the catalysts (including the type of active metal, metal particle size, acidity, pore size, the nature of the oxide supports, and the synergistic effect of the metals) are systematically reviewed based on the three most commonly used supports (carbon, oxides, and zeolites) in lignin hydrogenolysis. The catalytic performance (selectivity and yield of products) is evaluated, and the emerging catalytic mechanisms are introduced to better understand the catalyst design guidelines. Finally, based on the progress of existing studies, future directions for catalyst design in the field of lignin depolymerization are proposed.

Avoiding Sabatier's Limitation on Spatially Correlated Pt-Mn Atomic Pair Sites for Oxygen Electroreduction.

The development of highly active and low-cost oxygen reduction reaction (ORR) catalysts is crucial for the practical application of hydrogen fuel cells. However, the linear scaling relation (LSR) imposes an inherent Sabatier's limitation for most catalysts including the benchmark Pt with an insurmountable overpotential ceiling, impeding the development of efficient electrocatalysts. To avoid such a limitation, using earth-abundant metal oxides with different crystal phases as model materials, we propose an effective and dynamic reaction pathway through constructing spatially correlated Pt-Mn pair sites, achieving an excellent balance between high activity and low Pt loading. Experimental and theoretical calculations demonstrate that manipulating the intermetallic distance and charge distribution of Pt-Mn pairs can effectively promote O-O bond cleavage at these sites through a bridge configuration, circumventing the formation of *OOH intermediates. Meanwhile, the dynamic adsorption configuration transition from the bridge configuration of O2 to the end-on configuration of *OH improves *OH desorption at the Mn site within such pairs, thereby avoiding Sabatier's limitation. The well-designed Pt-Mn/ß-MnO2 exhibits outstanding ORR activity and stability with a half-wave potential of 0.93 V and barely any activity degradation for 70 h. When applied to the cathode of a H2-O2 anion-exchange membrane fuel cell, this catalyst demonstrates a high peak power density of 287 mW cm-2 and 500 h of stability under a cell voltage of 0.6 V. This work reveals the adaptive bonding interactions of atomic pair sites with multiple reactant/intermediates, offering a new avenue for rational design of highly efficient atomic-level dispersed ORR catalysts beyond the Sabatier optimum.

Progress in Manipulating Dynamic Surface Reconstruction via Anion Modulation for Electrocatalytic Water Oxidation.

The development of efficient and economical electrocatalysts for oxygen evolution reaction (OER) is of paramount importance for the sustainable production of renewable fuels and energy storage systems; however, the sluggish OER kinetics involving multistep four proton-coupled electron transfer hampers progress in these systems. Fortunately, surface reconstruction offers promising potential to improve OER catalyst design. Anion modulation plays a crucial role in controlling the extent of surface reconstruction and positively persuading the reconstructed species' performances. This review starts by providing a general explanation of how various types of anions can trigger dynamic surface reconstruction and create different combinations with pre-catalysts. Next, the influences of anion modulation on manipulating the surface dynamic reconstruction process are discussed based on the in situ advanced characterization techniques. Furthermore, various effects of survived anionic groups in reconstructed species on water oxidation activity are further discussed. Finally, the challenges and prospects for the future development directions of anion modulation for redirecting dynamic surface reconstruction to construct highly efficient and practical catalysts for water oxidation are proposed.

Reconstructed Ir‒O‒Mo species with strong Brønsted acidity for acidic water oxidation.

Surface reconstruction generates real active species in electrochemical conditions; rational regulating reconstruction in a targeted manner is the key for constructing highly active catalyst. Herein, we use the high-valence Mo modulated orthorhombic Pr3Ir1-xMoxO7 as model to activate lattice oxygen and cations, achieving directional and accelerated surface reconstruction to produce self-terminated Ir‒Obri‒Mo (Obri represents the bridge oxygen) active species that is highly active for acidic water oxidation. The doped Mo not only contributes to accelerated surface reconstruction due to optimized Ir‒O covalency and more prone dissolution of Pr, but also affords the improved durability resulted from Mo-buffered charge compensation, thereby preventing fierce Ir dissolution and excessive lattice oxygen loss. As such, Ir‒Obri‒Mo species could be directionally generated, in which the strong Brønsted acidity of Obri induced by remaining Mo assists with the facilitated deprotonation of oxo intermediates, following bridging-oxygen-assisted deprotonation pathway. Consequently, the optimal catalyst exhibits the best activity with an overpotential of 259 mV to reach 10 mA cmgeo-2, 50 mV lower than undoped counterpart, and shows improved stability for over 200 h. This work provides a strategy of directional surface reconstruction to constructing strong Brønsted acid sites in IrOx species, demonstrating the perspective of targeted electrocatalyst fabrication under in situ realistic reaction conditions.

Spin selection in atomic-level chiral metal oxide for photocatalysis.

The spin degree of freedom is an important and intrinsic parameter in boosting carrier dynamics and surface reaction kinetics of photocatalysis. Here we show that chiral structure in ZnO can induce spin selectivity effect to promote photocatalytic performance. The ZnO crystals synthesized using chiral methionine molecules as symmetry-breaking agents show hierarchical chirality. Magnetic circular dichroism spectroscopic and magnetic conductive-probe atomic force microscopic measurements demonstrate that chiral structure acts as spin filters and induces spin polarization in photoinduced carriers. The polarized carriers not only possess the prolonged carrier lifetime, but also increase the triplet species instead of singlet byproducts during reaction. Accordingly, the left- and right-hand chiral ZnO exhibit 2.0- and 1.9-times higher activity in photocatalytic O2 production and 2.5- and 2.0-times higher activities in contaminant photodegradation, respectively, compared with achiral ZnO. This work provides a feasible strategy to manipulate the spin properties in metal oxides for electron spin-related redox catalysis.

The adipose-derived stem cell peptide ADSCP2 alleviates hypertrophic scar fibrosis via binding with pyruvate carboxylase and remodeling the metabolic landscape.

AIM: The purpose of this study was to investigate the function and mechanism of a novel peptide derived from adipose-derived stem cell-conditioned medium (ADSC-CM). METHODS: Mass spectrometry was applied to identify expressed peptides in ADSC-CM obtained at different time points. The cell counting kit-8 assay and quantitative reverse transcription polymerase chain reactions were performed to screen the functional peptides contained within ADSC-CM. RNA-seq, western blot, a back skin excisional model of BALB/c mice, the peptide pull-down assay, rescue experiments, untargeted metabolomics, and mixOmics analysis were performed to thoroughly understand the functional mechanism of selected peptide. RESULTS: A total of 93, 827, 1108, and 631 peptides were identified in ADSC-CM at 0, 24, 48, and 72 h of conditioning, respectively. A peptide named ADSCP2 (DENREKVNDQAKL) derived from ADSC-CM inhibited collagen and ACTA2 mRNAs in hypertrophic scar fibroblasts. Moreover, ADSCP2 facilitated wound healing and attenuated collagen deposition in a mouse model. ADSCP2 bound with the pyruvate carboxylase (PC) protein and inhibited PC protein expression. Overexpressing PC rescued the reduction in collagen and ACTA2 mRNAs caused by ADSCP2. Untargeted metabolomics identified 258 and 447 differential metabolites in the negative and positive mode, respectively, in the ADSCP2-treated group. The mixOmics analysis, which integrated RNA-seq and untargeted metabolomics data, provided a more holistic view of the functions of ADSCP2. CONCLUSION: Overall, a novel peptide derived from ADSC-CM, named ADSCP2, attenuated hypertrophic scar fibrosis in vitro and in vivo, and the novel peptide ADSCP2 might be a promising drug candidate for clinical scar therapy.

Synergetic effect of Au nanoparticles and transition metal phosphides for enhanced hydrogen evolution from ammonia-borane.

The hydrogen evolution from ammonia borane is intriguing but challenging due to its sluggish kinetics. In this regard, the gold nanoparticles amalgamation with metal phosphides is speculated to be more efficient catalysts. Here, the catalysts Au/Ni2P and Au/CoP with the high synergetic effect of Au nanoparticles and metal phosphides were synthesized for ammonia borane hydrolysis. The activity of Au/Ni2P increases 4.8-fold (i.e., 0.08 to 0.40 L∙h-1) compared to pristine Ni2P, and the activity of Au/CoP increases 1.7-fold (i.e., 0.74 to 1.27 L∙h-1) compared to pristine CoP. This reveals that the synergetic effect of Auδ+ and (Ni2P) δ- is stronger than Auδ+ and (CoP) δ- which is manifested by XPS analysis. The kinetics exposes that the activation energy of Au/Ni2P (45.28 kJ∙mole-1) is greater than Au/CoP (31.45 kJ∙mole-1) and the TOF of Au/Ni2P is less than Au/CoP. This research work presents an effective approach for producing active sites of Auδ+ and (Ni2P & CoP) δ- for ammonia borane hydrolysis to enhance the H2 evolution rate.

IrO2 Nanoparticle-Decorated Ir-Doped W18O49 Nanowires with High Mass Specific OER Activity for Proton Exchange Membrane Electrolysis.

The oxygen evolution reaction (OER) severely limits the efficiency of proton exchange membrane (PEM) electrolyzers due to slow reaction kinetics. IrO2 is currently a commonly used anode catalyst, but its large-scale application is limited due to its high price and scarce reserves. Herein, we reported a practical strategy to construct an acid OER catalyst where Iridium oxide loading and iridium element bulk doping are realized on the surface and inside of W18O49 nanowires by immersion adsorption, respectively. Specifically, W0.7Ir0.3Oy has an overpotential of 278 mV at 10 mA·cm-2 in 0.1 M HClO4. The mass activity of 714.10 A·gIr-1 at 1.53 V vs. the reversible hydrogen electrode (RHE) is 80 times that of IrO2, and it can run stably for 55 h. In the PEM water electrolyzer device, its mass activity reaches 3563.63 A·gIr-1 at the cell voltage of 2.0 V. This improved catalytic performance is attributed to the following aspects: (1) The electron transport between iridium and tungsten effectively improves the electronic structure of the catalyst; (2) the introduction of iridium into W18O49 by means of elemental bulk doping and nanoparticles supporting for the enhanced conductivity and electrochemically active surface area of the catalyst, resulting in extensive exposure of active sites and increased intrinsic activity; and (3) during the OER process, partial iridium elements in the bulk phase are precipitated, and iridium oxide is formed on the surface to maintain stable activity. This work provides a new idea for designing oxygen evolution catalysts with low iridium content for practical application in PEM electrolyzers.

Tracking the Role of Defect Types in Co3O4 Structural Evolution and Active Motifs during Oxygen Evolution Reaction.

Dynamic reconstruction of catalyst active sites is particularly important for metal oxide-catalyzed oxygen evolution reaction (OER). However, the mechanism of how vacancy-induced reconstruction aids OER remains ambiguous. Here, we use Co3O4 with Co or O vacancies to uncover the effects of different defects in the reconstruction process and the active motifs relevant to alkaline OER. Combining in situ characterization and theoretical calculations, we found that cobalt oxides are converted to an amorphous [Co(OH)6] intermediate state, and then the mismatched rates of *OH adsorption and deprotonation lead to irreversible catalyst reconstruction. The stronger *OH adsorption but weaker deprotonation induced by O defects provides the driving force for reconstruction, while Co defects favor dehydrogenation and reduce the reconstruction rate. Importantly, both O and Co defects trigger highly OER-active bridge Co sites in reconstructed catalysts, of which Co defects induce a short Co-Co distance (3.38 Å) under compressive lattice stress and show the best OER activity (η10 of 262 mV), superior to reconstructed oxygen-defected Co3O4-VO (η10 of 300 mV) and defect-free Co3O4 (η10 of 320 mV). This work highlights that engineering defect-dependent reconstruction may provide a rational route for electrocatalyst design in energy-related applications.