Suppressed Ion Migration in FA-Rich Perovskite Photovoltaics through Enhanced Nucleation of Encapsulation Interface.

With excellent homogeneity, compactness and controllable thickness, atomic layer deposition (ALD) technology is widely used in perovskite solar cells (PSCs). However, residual organic sources and undesired reactions pose serious challenges to device performance as well as stability. Here, ester groups of poly(ethylene-co-vinyl acetate) are introduced as a reaction medium to promote the nucleation and complete conversion of tetrakis(dimethylamino)tin(IV) (TDMA-Sn). Through simulations and experiments, it is verified that ester groups as Lewis bases can coordinate with TDMA-Sn to facilitate homogeneous deposition of ALD-SnOx , which acts as self-encapsulated interface with blocking properties against external moisture as well as internal ion migration. Meanwhile, a comprehensive evaluation of the self-encapsulated interface reveals that the energy level alignment is optimized to improve the carrier transport. Finally, the self-encapsulated device obtains a champion photovoltaic conversion efficiency (PCE) of 22.06% and retains 85% of the initial PCE after being stored at 85 °C with relative humidity of 85% for more than 800 h.

Unlocking the Effect of Chain Length and Terminal Group on Ethylene Glycol Ether Family Toward Advanced Aqueous Electrolytes.

Constructing high-performance hybrid electrolyte is important to advanced aqueous electrochemical energy storage devices. However, due to the lack of in-depth understanding of how the molecule structures of cosolvent additives influence the properties of electrolytes significantly impeded the development of hybrid electrolytes. Herein, a series of hybrid electrolytes are prepared by using ethylene glycol ether with different chain lengths and terminal groups as additives. The optimized 2 m LiTFSI-90%DDm hybrid electrolyte prepared from diethylene glycol dimethyl ether (DDm) molecule showcases excellent comprehensive performance and significantly enhances the operating voltage of supercapacitors (SCs) to 2.5 V by suppressing the activity of water. Moreover, the SC with 2 m LiTFSI-90%DDm hybrid electrolyte supplies a long-term cycling life of 50 000 cycles at 1 A g-1 with 92.3% capacitance retention as well as excellent low temperature (-40 ºC) cycling performance (10 000 times at 0.2 A g-1). Universally, Zn//polyaniline full cell with 2 m Zn(OTf)2-90%DDm electrolyte manifests outstanding cycling performance in terms of 77.9% capacity retention after 2,000 cycles and a dendrite-free Zn anode. This work inspires new thinking of developing advanced hybrid electrolytes by cosolvent molecule design toward high-performance energy storage devices.

A Self-Assembled 3D/0D Quasi-Core-Shell Structure as Internal Encapsulation Layer for Stable and Efficient FAPbI3 Perovskite Solar Cells and Modules.

FAPbI3 perovskites have garnered considerable interest owing to their outstanding thermal stability, along with near-theoretical bandgap and efficiency. However, their inherent phase instability presents a substantial challenge to the long-term stability of devices. Herein, this issue through a dual-strategy of self-assembly 3D/0D quasi-core-shell structure is tackled as an internal encapsulation layer, and in situ introduction of excess PbI2 for surface and grain boundary defects passivating, therefore preventing moisture intrusion into FAPbI3 perovskite films. By utilizing this method alone, not only enhances the stability of the FAPbI3 film but also effectively passivates defects and minimizes non-radiative recombination, ultimately yielding a champion device efficiency of 23.23%. Furthermore, the devices own better moisture resistance, exhibiting a T80 lifetime exceeding 3500 h at 40% relative humidity (RH). Meanwhile, a 19.51% PCE of mini-module (5 × 5 cm2) is demonstrated. This research offers valuable insights and directions for the advancement of stable and highly efficient FAPbI3 perovskite solar cells.

Performance evaluation of core genome multilocus sequence typing for genotyping of Mycobacterium tuberculosis strains in China: based on multicenter, population-based collection.

PURPOSE: To evaluate the performance of core genome multilocus sequence typing (cgMLST) for genotyping Mycobacterium tuberculosis (M.tuberculosis) Strains in regions where the lineage 2 strains predominate. METHODS: We compared clustering by whole-genome SNP typing with cgMLST clustering in the analysis of WGS data of 6240 strains from five regions of China. Using both the receiver operating characteristic (ROC) curve and epidemiological investigation to determine the optimal threshold for defining genomic clustering by cgMLST. The performance of cgMLST was evaluated by quantifying the sensitivity, specificity and concordance of clustering between two methods. Logistic regression was used to gauge the impact of strain genetic diversity and lineage on cgMLST clustering. RESULTS: The optimal threshold for cgMLST to define genomic clustering was determined to be ≤ 10 allelic differences between strains. The overall sensitivity and specificity of cgMLST averaged 99.6% and 96.3%, respectively; the concordance of clustering between two methods averaged 97.1%. Concordance was significantly correlated with strain genetic diversity and was 3.99 times (95% CI, 2.94-5.42) higher in regions with high genetic diversity (π > 1.55 × 10-4) compared to regions with low genetic diversity. The difference missed statistical significance, while concordance for lineage 2 strains (96.8%) was less than that for lineage 4 strains (98.3%). CONCLUSION : cgMLST showed a discriminatory power comparable to whole-genome SNP typing and could be used to genotype clinical M.tuberculosis strains in different regions of China. The discriminative power of cgMLST was significantly correlated with strain genetic diversity and was slightly lower with strains from regions with low genetic diversity.

Spontaneous Internal Encapsulation via Dual Interfacial Perovskite Heterojunction Enables Highly Efficient and Stable Perovskite Solar Cells.

Deep traps stemming from the defects formed at the surfaces and grain boundaries of the perovskite films are the main reasons of nonradiative recombination and material degradation, which significantly affect efficiency and stability of perovskite solar cells (PSCs). Here, a spontaneous internal encapsulation strategy was developed by constructing a dual interfacial perovskite heterojunction at the top and buried interface of the three-dimensional (3D) perovskite film. The spacer cations of the two-dimensional (2D) perovskite structure interacted strongly with the 3D perovskite to passivate the defects and optimize the energy level alignment. Meanwhile, the interfacial perovskite heterojunction underearth delayed the crystallization speed and improved the crystallization quality of the upper 3D perovskite. Thanks to these positive effects, the PSC exhibited a power conversion efficiency of 22.92% with good reproducibility. Significantly, the unencapsulated device with the dual interfacial perovskite heterojunction maintained 88% of its initial efficiency after 2900 h under 65 ± 5% RH in air.

Synchronous Elimination of Excess Photoinstable PbI2 and Interfacial Band Mismatch for Efficient and Stable Perovskite Solar Cells.

Eliminating the undesired photoinstability of excess lead iodide (PbI2 ) in the perovskite film and reducing the energy mismatch between the perovskite layer and heterogeneous interfaces are urgent issues to be addressed in the preparation of perovskite solar cells (PVSCs) by two-step sequential deposition method. Here, the 1-ethyl-3-methylimidazolium tetrafluoroborate (EMIMBF4 ) is employed to convert superfluous PbI2 to more robust 1D EMIMPbI3 which can withstand lattice strain, while forming an interfacial dipole layer at the SnO2 /perovskite interface to reconfigure the interfacial energy band structure and accelerate the charge extraction. Consequently, the unencapsulated PVSCs device attains a champion efficiency of 24.28 % with one of the highest open-circuit voltage (1.19 V). Moreover, the unencapsulated devices showcase significantly improved thermal stability, enhanced environmental stability and remarkable operational stability accompanied by 85 % of primitive efficiency retained over 1500 h at maximum power point tracking under continuous illumination.

Regulating Charge Transport Dynamics at the Buried Interface and Bulk of Perovskites by Tailored-phase Two-dimensional Crystal Seed Layer.

Targeting the trap-assisted non-radiative recombination losses and photochemical degradation occurring at the interface and bulk of perovskite, especially the overlooked buried bottom interface, a strategy of tailored-phase two-dimensional (TP-2D) crystal seed layer has been developed to improve the charge transport dynamics at the buried interface and bulk of perovskite films. Using this approach, TP-2D layer constructed by TP-2D crystal seeds at the buried interface can induce the formation of homogeneous interface electric field, which effectively suppress the accumulation of charge carriers at the buried interface. Additionally, the presence of TP-2D crystal seed has a positive effect on the crystallization process of the upper perovskite film, leading to optimized crystal quality and thus promoted charge transport inside bulk perovskites. Ultimately, the best performing PSCs based on TP-2D layer deliver a power conversion efficiency of 24.58 %. The devices exhibit an improved photostability with 88.4 % of their initial PCEs being retained after aging under continuous 0.8-sun illumination for 2000 h in air. Our findings reveal how to regulate the charge transport dynamics of perovskite bulk and interface by introducing homogeneous components.

Amine-releasable Mediator In situ Repair Perovskites for Efficient and Stable Perovskite Solar Cells.

Residual lead iodide (PbI2) is deemed to a double-edged sword in perovskite film as small amounts of PbI2 are beneficial to the photovoltaic performance, but excessive will cause degradation of photovoltaic performance and stability. Herein, an in situ repair strategy has been developed by introducing amine-releasable mediator (methylammonium pyridine-2-carboxylic, MAPyA) to eliminate over-residual PbI2 and regulate the crystal quality of perovskite film. Notably, MAPyA can be partially decomposed into methylamine (MA) gas and pyridine-2-carboxylic (PyA) during high temperature annealing. The released MA can locally form liquid intermediate phase, facilitating the reconstruction of perovskite microcrystals and residual PbI2. Moreover, the leftover PyA is confirmed to effectively passivate the uncoordinated lead ions in final perovskite film. Based upon this, superior perovskite film with optimized crystal structure and holistic negligible PbI2 is acquired. The assembled device realizes outstanding efficiency of 24.06 %, and exhibits a remarkable operational stability that maintaining 87 % of its origin efficiency after continuous illumination for 1480 h. And the unencapsulated MAPyA-treated devices present significant uplift in humidity stability (maintaining ~93 % of the initial efficiency over 1500 h, 50-60 % relative humidity). Furthermore, the further optimization of this strategy with nanoimprint technology proves its superiority in the amplificative preparation for perovskite films.

Multifunctional Cellulose Nanocrystals Electrolyte Additive Enable Ultrahigh-Rate and Dendrite-Free Zn Anodes for Rechargeable Aqueous Zinc Batteries.

The design of aqueous zinc (Zn) chemistry energy storage with high rate-capability and long serving life is a great challenge due to its inhospitable coordination environment and dismal interfacial chemistry. To bridge this big gap, herein, we build a highly reversible aqueous Zn battery by taking advantages of the biomass-derived cellulose nanocrystals (CNCs) electrolyte additive with unique physical and chemical characteristics simultaneously. The CNCs additive not only serves as fast ion carriers for enhancing Zn2+ transport kinetics but regulates the coordination environment and interface chemistry to form dynamic and self-repairing protective interphase, resulting in building ultra-stable Zn anodes under extreme conditions. As a result, the engineered electrolyte system achieves a superior average coulombic efficiency of 97.27 % under 140 mA cm-2, and steady charge-discharge for 982 h under 50 mA cm-2, 50 mAh cm-2, which proposes a universal pathway to challenge aqueous Zn chemistry in green, sustainable, and large-scale applications.

Regulating Crystallinity Mismatch Between Donor and Acceptor to Improve Exciton/Charge Transport in Efficient Organic Solar Cells.

Achieving a more balanced charge transport by morphological control is crucial in reducing bimolecular and trap-assisted recombination and enhancing the critical parameters for efficient organic solar cells (OSCs). Hence, a facile strategy is proposed to reduce the crystallinity difference between donor and acceptor by incorporating a novel multifunctional liquid crystal small molecule (LCSM) BDTPF4-C6 into the binary blend. BDTPF4-C6 is the first LCSM based on a tetrafluorobenzene unit and features a low liquid crystal phase transition temperature and strong self-assembly ability, conducive to regulating the active layer morphology. When BDTPF4-C6 is introduced as a guest molecule into the PM6 : Y6 binary, it exhibits better compatibility with the donor PM6 and primarily resides within the PM6 phase because of the similarity-intermiscibility principle. Moreover, systematic studies revealed that BDTPF4-C6 could be used as a seeding agent for PM6 to enhance its crystallinity, thereby forming a more balanced and favourable charge transport with suppressed charge recombination. Intriguingly, dual Förster resonance energy transfer was observed between the guest molecule and the host donor and acceptor, resulting in an improved current density. This study demonstrates a facile approach to balance the charge mobilities and offers new insights into boosting the efficiency of single-junction OSCs beyond 20 %.

Dual-Strategy Tailoring Molecular Structures of Dopant-Free Hole Transport Materials for Efficient and Stable Perovskite Solar Cells.

Dopant-free hole transport materials (HTMs) are ideal materials for highly efficient and stable n-i-p perovskite solar cells (PSCs), but most current design strategies for tailoring the molecular structures of HTMs are limited to single strategy. Herein, four HTMs based on dithienothiophenepyrrole (DTTP) core are devised through dual-strategy methods combining conjugate engineering and side chain engineering. DTTP-ThSO with ester alkyl chain that can form six-membered ring by the S⋅⋅⋅O noncovalent conformation lock with thiophene in the backbone shows good planarity, high-quality film, matching energy level and high hole mobility, as well as strong defect passivation ability. Consequently, a remarkable power conversion efficiency (PCE) of 23.3 % with a nice long-term stability is achieved by dopant-free DTTP-ThSO-based PSCs, representing one of the highest values for un-doped organic HTMs based PSCs. Especially, the fill factor (FF) of 82.3 % is the highest value for dopant-free small molecular HTMs-based n-i-p PSCs to date. Moreover, DTTP-ThSO-based devices have achieved an excellent PCE of 20.9 % in large-area (1.01 cm2) devices. This work clearly elucidates the structure-performance relationships of HTMs and offers a practical dual-strategy approach to designing dopant-free HTMs for high-performance PSCs.

Over 19 % Efficiency Organic Solar Cells Enabled by Manipulating the Intermolecular Interactions through Side Chain Fluorine Functionalization.

Fluorine side chain functionalization of non-fullerene acceptors (NFAs) represents an effective strategy for enhancing the performance of organic solar cells (OSCs). However, a knowledge gap persists regarding the relationship between structural changes induced by fluorine functionalization and the resultant impact on device performance. In this work, varying amounts of fluorine atoms were introduced into the outer side chains of Y-series NFAs to construct two acceptors named BTP-F0 and BTP-F5. Theoretical and experimental investigations reveal that side-chain fluorination significantly increase the overall average electrostatic potential (ESP) and charge balance factor, thereby effectively improving the ESP-induced intermolecular electrostatic interaction, and thus precisely tuning the molecular packing and bulk-heterojunction morphology. Therefore, the BTP-F5-based OSC exhibited enhanced crystallinity, domain purity, reduced domain spacing, and optimized phase distribution in the vertical direction. This facilitates exciton diffusion, suppresses charge recombination, and improves charge extraction. Consequently, the promising power conversion efficiency (PCE) of 17.3 % and 19.2 % were achieved in BTP-F5-based binary and ternary devices, respectively, surpassing the PCE of 16.1 % for BTP-F0-based OSCs. This work establishes a structure-performance relationship and demonstrates that fluorine functionalization of the outer side chains of Y-series NFAs is a compelling strategy for achieving ideal phase separation for highly efficient OSCs.

Transcriptomic Analysis of Mycobacterial Infected Macrophages Reveals a High MOI Specific Type I IFN Signaling.

Macrophage (MΦ) infection models are important tools for studying host-mycobacterial interactions. Although the multiplicity of infection (MOI) is an important experimental variable, the selection of MOI in mycobacterial infection experiments is largely empirical, without reference to solid experimental data. To provide relevant data, we used RNA-seq to analyze the gene expression profiles of MΦs 4 or 24 h after infection with Mycobacterium marinum (M. m) at MOIs ranging from 0.1 to 50. Analysis of differentially expressed genes (DEGs) showed that different MOIs are linked to distinct transcriptomic changes and only 10% of DEGs were shared by MΦ infected at all MOIs. KEGG pathway enrichment analysis revealed that type I interferon (IFN)-related pathways were inoculant dose-dependent and enriched only at high MOIs, whereas TNF pathways were inoculant dose-independent and enriched at all MOIs. Protein-protein interaction (PPI) network alignment showed that different MOIs had distinct key node genes. By fluorescence-activated cell sorting and follow-up RT-PCR analysis, we could separate infected MΦs from uninfected MΦs and found phagocytosis of mycobacteria to be the determinant factor for type I IFN production. The distinct transcriptional regulation of RAW264.7 MΦ genes at different MOIs was also seen with Mycobacterium tuberculosis (M.tb) infections and primary MΦ infection models. In summary, transcriptional profiling of mycobacterial infected MΦs revealed that different MOIs activate distinct immune pathways and the type I IFN pathway is activated only at high MOIs. This study should provide guidance for selecting the MOI most appropriate for different research questions.

Halogen-Free Donor Polymers Based on Dicyanobenzotriazole with Low Energy Loss and High Efficiency in Organic Solar Cells.

Halogenation of organic semiconductors is an efficient strategy for improving the performance of organic solar cells (OSCs), while the introduction of halogens usually involves complex synthetic process and serious environment pollution problems. Herein, three halogen-free ternary copolymer donors (PCNx, x = 3, 4, 5) based on electron-withdrawing dicyanobenzotriazole are reported. When blended with the Y6, PCN3 with strong interchain interactions results in appropriate crystallinity and thermodynamic miscibility of the blend film. Grazing-incidence wide-angle X-ray scattering measurements indicate that PCN3 has more ordered arrangement and stronger π-π stacking than previous PCN2. Fourier-transform photocurrent spectroscopy and external quantum efficiency of electroluminescence measurements show that PCN3-based OSCs have lower energy loss than PCN2, which leads to their higher open-circuit voltage (0.873 V). The device based on PCN3 reaches power conversion efficiency (PCE) of 15.33% in binary OSCs, one of the highest values for OSCs with halogen-free donor polymers. The PCE of 17.80% and 18.10% are obtained in PM6:PCN3:Y6 and PM6:PCN3:BTP-eC9 ternary devices, much higher than those of PM6:Y6 (16.31%) and PM6:BTP-eC9 (17.33%) devices. Additionally, this ternary OSCs exhibit superior stability compared to binary host system. This work gives a promising path for halogen-free donor polymers to achieve low energy loss and high PCE.

Disentangling the Li-Ion transport and Boundary Phase Transition Processes in Li10 GeP2 S12 Electrolyte by In-Operando High-Pressure and High-Resolution NMR Spectroscopy.

Li-ion transport and phase transition of solid electrolytes are critical and fundamental issues governing the rate and cycling performances of solid-state batteries. In this work, in-operando high-pressure nuclear magnetic resonance (NMR) spectroscopy for the solid-state battery is developed and applied, in combination with 6 Li-tracer NMR and high-resolution NMR spectroscopy, to investigate the Li10 GeP2 S12 electrolyte under true-to-life operation conditions. The results reveal that the Li10 GeP2 S12 phase may become more disordered and a large amount of conductive metastable ß-Li3 PS4 as the glassy matrix in the electrolyte transforms into less conductive phases, mainly γ-Li3 PS4 , when high current densities (e.g., ≥0.5 mA cm-2 ) are applied to the electrolyte. The overall Li-transport also varies and shows a tendency of boundary phases and Li10 GeP2 S12 synergistic dominant conduction at high currents. Accordingly, a mechanism of structural change induced by stress variation due to the drastic morphological change during Li-In alloying at high currents, and the local Li+ diffusion coefficient discrepancy is proposed. These new findings of Li-ion transport and boundary phase transition in Li10 GeP2 S12 solid electrolyte under high-pressure and high current density are first reported and will help provide previously lacking insights into the relationship of structure and performance of Li10 GeP2 S12 .

Disentangling Phase and Morphological Evolution During the Formation of the Lithium Superionic Conductor Li10 GeP2 S12.

The structural and morphological changes of the Lithium superionic conductor Li10 GeP2 S12 , prepared via a widely used ball milling-heating method over a comprehensive heat treatment range (50 - 700 °C), are investigated. Based on the phase composition, the formation process can be distinctly separated into four zones: Educt, Intermediary, Formation, and Decomposition zone. It is found that instead of Li4 GeS4 -Li3 PS4 binary crystallization process, diversified intermediate phases, including GeS2 in different space groups, multiphasic lithium phosphosulfides (Lix Py Sz ), and cubic Li7 Ge3 PS12 phase, are involved additionally during the formation and decomposition of Li10 GeP2 S12 . Furthermore, the phase composition at temperatures around the transition temperatures of different formation zones shows a significant deviation. At 600 °C, Li10 GeP2 S12 is fully crystalline, while the sample decomposed to complex phases at 650 °C with 30 wt.% impurities, including 20 wt.% amorphous phases. These findings over such a wide temperature range are first reported and may help provide previously lacking insights into the formation and crystallinity control of Li10 GeP2 S12 .

Polycation-Regulated Electrolyte and Interfacial Electric Fields for Stable Zinc Metal Batteries.

Zn metal as one of promising anode materials for aqueous batteries but suffers from disreputable dendrite growth, grievous hydrogen evolution and corrosion. Here, a polycation additive, polydiallyl dimethylammonium chloride (PDD), is introduced to achieve long-term and highly reversible Zn plating/stripping. Specifically, the PDD can simultaneously regulate the electric fields of electrolyte and Zn/electrolyte interface to improve Zn2+ migration behaviors and guide dominant Zn (002) deposition, which is veritably detected by Zeta potential, Kelvin probe force microscopy and scanning electrochemical microscopy. Moreover, PDD also creates a positive charge-rich protective outer layer and a N-rich hybrid inner layer, which accelerates the Zn2+ desolvation during plating process and blocks the direct contact between water molecules and Zn anode. Thereby, the reversibility and long-term stability of Zn anodes are substantially improved, as certified by a higher average coulombic efficiency of 99.7 % for Zn||Cu cells and 22 times longer life for Zn||Zn cells compared with that of PDD-free electrolyte.

Electron-Donors-Acceptors Interaction Enhancing Electrocatalytic Activity of Metal-Organic Polymers for Oxygen Reduction.

Catalysts with metal-Nx sites have long been considered as effective electrocatalysts for oxygen reduction reaction (ORR), yet the accurate structure-property correlations of these active sites remain debatable. Report here is a proof-of-concept method to construct 1,4,8,11-tetraaza[14]annulene (TAA)-based polymer nanocomposites with well-managed electronic microenvironment via electron-donors/acceptors interaction of altering electron-withdrawing ß-site substituents. DFT calculation proves the optimal -Cl substituted catalyst (CoTAA-Cl@GR) tailored the key OH* intermediate interaction with Co-N4 sites under the d-orbital regulation, hence reaching the top of ORR performance with excellent turnover frequency (0.49 e s-1 site-1 ). The combination of in situ scanning electrochemical microscopy and variable-frequency square wave voltammetry techniques contribute the great ORR kinetics of CoTAA-Cl@GR to the relatively high accessible site density (7.71×1019  site g-1 ) and fast electron outbound propagation mechanism. This work provides theoretical guidance for rational design of high-performance catalysts for ORR and beyond.

Uncovering Aging Chemistry of Perovskite Precursor Solutions and Anti-aging Mechanism of Additives.

The aging of precursor solutions is the major stumbling block for the commercialization of perovskite solar cells (PSCs). Herein, for the first time we used the state-of-the-art in situ liquid time-of-flight secondary ion mass spectrometry to molecularly explore the perovskite precursor solution chemistry. We identified that the methylammonium and formamidinium cations and the I- anion are the motivators of the aging chemistry. Further, we introduced two kinds of Lewis bases, triethyl phosphate (TP) and ethyl ethanesulfonate (EE), as new additives in the solution and unraveled that both of them can protect the reactive cations from aging through weak interactions. Significantly, TP is superior to EE in enhancing long-term solution stability as it can well-maintain the internal interaction structures within the solution phase. The PSC derived from a fresh TP-doped solution delivered a high power conversion efficiency of 23.06 %, 92.23 % of which remained in that from a 21-day-old solution.

Longitudinally Grafting of Graphene with Iron Phthalocyanine-based Porous Organic Polymer to Boost Oxygen Electroreduction.

Iron phthalocyanine-based polymers (PFePc) are attractive noble-metal-free candidates for catalyzing oxygen reduction reaction (ORR). However, the low site-exposure degree and poor electrical conductivity of bulk PFePc restricted their practical applications. Herein, laminar PFePc nanosheets covalently and longitudinally linked to graphene (3D-G-PFePc) was prepared. Such structural engineering qualifies 3D-G-PFePc with high site utilization and rapid mass transfer. Thence, 3D-G-PFePc demonstrates efficient ORR performance with a high specific activity of 69.31 µA cm-2 , a high mass activity of 81.88 A g-1 , and a high turnover frequency of 0.93 e s-1 site-1 at 0.90 V vs. reversible hydrogen electrode in O2 -saturated 0.1 M KOH, outperforming the lamellar PFePc wrapped graphene counterpart. Systematic electrochemical analyses integrating variable-frequency square wave voltammetry and in situ scanning electrochemical microscopy further underline the rapid kinetics of 3D-G-PFePc towards ORR.