Two Birds One Stone: Graphene Assisted Reaction Kinetics and Ionic Conductivity in Phthalocyanine-Based Covalent Organic Framework Anodes for Lithium-ion Batteries

This work reports a covalent organic framework composite structure (PMDA-NiPc-G), incorporating multiple-active carbonyls and graphene on the basis of the combination of phthalocyanine (NiPc(NH₂)₄) containing a large π-conjugated system and pyromellitic dianhydride (PMDA) as the anode of lithium-ion batteries. Meanwhile, graphene is used as a dispersion medium to reduce the accumulation of bulk covalent organic frameworks (COFs) to obtain COFs with small-volume and few-layers, shortening the ion migration path and improving the diffusion rate of lithium ions in the two dimensional (2D) grid layered structure. PMDA-NiPc-G showed a lithium-ion diffusion coefficient (D_Li⁺) of 3.04 × 10⁻¹⁰ cm² s⁻¹ which is 3.6 times to that of its bulk form (0.84 × 10⁻¹⁰ cm² s⁻¹). Remarkably, this enables a large reversible capacity of 1290 mAh g⁻¹ can be achieved after 300 cycles and almost no capacity fading in the next 300 cycles at 100 mA g⁻¹. At a high areal capacity loading of ≈3 mAh cm⁻², full batteries assembled with LiNi_0.8Co_0.1Mn_0.1O₂ (NCM-811) and LiFePO₄ (LFP) cathodes showed 60.2% and 74.7% capacity retention at 1 C for 200 cycles. Astonishingly, the PMDA-NiPc-G/NCM-811 full battery exhibits ≈100% capacity retention after cycling at 0.2 C. Aided by the analysis of kinetic behavior of lithium storage and theoretical calculations, the capacity-enhancing mechanism and lithium storage mechanism of covalent organic frameworks are revealed. This work may lead to more research on designable, multifunctional COFs for electrochemical energy storage.     

Constructing the high-areal-capacity,solid-state Li polymer battery via the multiscale ion transport pathway design

The parasitic Li dendrite formation and retarded ion diffusion dynamics inhibit the deployment of solid-state batteries (SSBs) at high areal capacity loadings. Here, we present the modular design of the Li⁺ percolating network by grafting the ionic-conductive polyether amine (PEA) at the multiple scales: the PEA modified zinc hydroxystannate (PEA@ZHS) (flame retardant units) and polyamide 6 (mechanical rigid units) are coherently introduced to optimize the PEO-based solid electrolyte (PX-PEA@ZHS) with the Young's modulus (3.41 GPa), ionic conductivity (4.29 × 10⁻⁴ S cm⁻¹ at 55 °C) and flame retardancy (22% reduction of heat release rate); on the other hand, PEA molecules are grafted onto the acetylene black additive to establish the dual conductive network, endowing two orders of magnitude increase of ionic conductivity for the high-compaction cathodes. The as-integrated symmetric cell exhibits a critical current density up to 0.8 mA cm⁻² and cycling endurance for 1000 h at 0.2 mA cm⁻²; upon the SSBs assembly with the record high loading of LiFePO₄ (12.4 mg cm⁻²), the high-areal-capacity, cycling stability as well as the extreme temperature endurance till 110 °C are simultaneously realized, which inspire the rational design of commercially feasible, energy-dense, flame-resistance energy storage prototype.     

Engineering Interfacial Built-in Electric Field in Polymetallic Phosphide Heterostructures for Superior Supercapacitors and Electrocatalytic Hydrogen Evolution

Herein, a patterned rod-like CoP@NiCoP core-shell heterostructure is designed to consist of CoP nanowires cross-linked with NiCoP nanosheets in tight strings. The interfacial interaction within the heterojunction between the two components generates a built-in electric field that adjusts the interfacial charge state and create more active sites, accelerating the charge transfer and improving supercapacitor and electrocatalytic performance. The unique core-shell structure suppresses the volume expansion during charging and discharging, achieving excellent stability. As a result, CoP@NiCoP exhibits a high specific capacitance of 2.9 F cm⁻² at a current density of 3 mA cm⁻² and a high ion diffusion rate (D_ion is 2.95 × 10⁻¹⁴ cm² s⁻¹) during charging/discharging. The assembled asymmetric supercapacitor CoP@NiCoP//AC exhibits a high energy density of 42.2 Wh kg⁻¹ at a power density of 126.5 W kg⁻¹ and excellent stability with a capacitance retention rate of 83.8% after 10 000 cycles. Furthermore, the modulated effect induced by the interfacial interaction also endows the self-supported electrode with excellent electrocatalytic HER performance with an overpotential of 71 mV at 10 mA cm⁻². This research may provide a new perspective on the generation of built-in electric field through the rational design of heterogeneous structures for improving the electrochemical and electrocatalytical performance.     

Neutron flux measurements with a Li2B4O7 crystal

The effect of neutron irradiation on a lithium tetraborate (Li₂B₄O₇, LBO) single crystal has been investigated. The crystals of high optical quality are found to be quite stable under high neutron fluence. This study shows that LBO crystals can be used as a proportional counter for neutron fluxes of the order 10⁹ cm⁻² s⁻¹ and higher. The detectors fabricated were found to have a sensitivity of ∼3×10⁻¹⁸ A (nv)⁻¹.     

Centimeter-Sized Single Crystals of Dion-Jacobson Phase Lead-Free Double Perovskite for Efficient X-ray Detection

2D Dion–Jacobson (DJ) phase hybrid perovskites have shown great promise in the photoelectronic field owing to their outstanding optoelectronic performance and superior structural rigidity. However, DJ phase lead-free double perovskites are still a virgin land with direct X-ray detection. Herein, we have designed and synthesized a new DJ phase lead-free layered double perovskite of (HIS)₂AgSbBr₈ ( 1 , HIS²⁺ = histammonium). Centimeter-sized (18 × 10 × 5 mm³) single crystals of 1 are successfully grown via the temperature cooling technique, exhibiting remarkable semiconductive characteristics such as a high resistivity (2.2 × 10¹¹ Ω cm), a low trap state density (3.56 × 10¹⁰ cm⁻³), and a large mobility-lifetime product (1.72 × 10⁻³ cm² V⁻¹). Strikingly, its single-crystal-based X-ray detector shows a high sensitivity of 223 µC Gy⁻¹_air cm⁻² under 33.3 V mm⁻¹, a low detection limit (84.2 nGy_airs⁻¹) and superior anti-fatigue. As far as we know, we firstly demonstrates the potential of 2D DJ phase lead-free hybrid double perovskite in X-ray detection, showing excellent photoelectric response and operational stability. This work will pave a promising pathway to the innovative application of hybrid perovskites for eco-friendly and efficient X-ray detection.     

Low-temperature synthesis of CeB6 nanowires and nanoparticles as feasible lithium-ion anode materials

Metallic CeB₆ nanomaterials were prepared via the low-temperature solution combustion method (nanoparticles) and high-pressure solid state reaction (nanowires). X-ray diffraction patterns and High-resolution transmission electron microscopy images reveal that CeB₆ nanoparticles are highly crystalline and CeB₆ nanowires are single crystals. The X-ray photoelectron spectroscopy analysis indicates that the cerium is present in the +3 and +4 mixed-valence state in CeB₆. As lithium-ion anodes, CeB₆ nanowires (nanoparticles) electrode achieves a capacity of ~531 (338) mA h g⁻¹ in the initial cycle and keeps a reversible capacity of ~225 (185) mA h g⁻¹ after 60 cycles. CeB₆ nanowires are tested for 6000 cycles at 1000 mA g⁻¹, which shows a specific capacity approaching to the capacity at 100 mA g⁻¹ in spite of fluctuation within a narrow range, and keep ~168 mA h g⁻¹ after 6000 cycles, indicating a stable cycling performance owing to the excellent metal-like conductivity of (~5.67 × 10³ S m⁻¹). The reason of capacity rising is that the reduction and oxidation levels of CeB₆ electrodes are improved after the 2nd cycle with Li⁺ insertion/extraction. Meanwhile, kinetic analysis reveals that the Li⁺ storage mechanism is mainly controlled by a surface capacitive behavior.     

High performance of LiFePO4 with nitrogen-doped carbon layers for lithium ion batteries

Herein, we demonstrate a facile approach to fabricate a cathode material of LiFePO₄ with nitrogen-doped carbon layers by applying egg white as both carbon source and nitrogen sources. The nitrogen doped carbon layers are in situ coated on the LiFePO₄ particles, which effectively improves the electrical conductivity of rapid Li-ion diffusion. When evaluated as a cathode material for lithium ion batteries (LIBs), LiFePO₄ material with nitrogen doped carbon shows high capacities of 164 mA h g⁻¹ at 0.1 C, 144 mA h g⁻¹ at 1 C and 120 mA h g⁻¹ at 5 C. The result implies that such novel LiFePO₄ material is a potential cathode material for LIBs.     

Matching CP@NCOH/NF Cathode and GH/FNP/NF Anode for High-Performance Asymmetric Supercapacitor

It is extremely crucial to design and match high-quality cathode and anode for achieving high-performance asymmetric supercapacitors (ASCs). Herein, Co₃(PO₄)₂@NiCo-LDH/Ni foam (CP@NCOH/NF) cathode with hierarchical morphology and graphene hydrogel/Fe–Ni phosphide/Ni foam (GH/FNP/NF) anode with the robust and porous structure are elaborately designed and prepared, respectively. Owing to their unique and profitable structures, both CP@NCOH/NF and GH/FNP/NF electrodes yield the superior capacity (10760 and 2236 mC cm⁻² at 2 mA cm⁻², respectively), good rate capability (63% retention at 200 mA cm⁻² and 52% retention at 50 mA cm⁻², respectively), and excellent cycling stability (72% and 74% retention after 10 000 cycles, respectively). Benefiting from their matchable electrochemical performances, the configured solid-state CP@NCOH/NF//GH/FNP/NF ASC outputs both competitive energy density (80.2 Wh kg⁻¹/4.1 mWh cm⁻³) and power density (14563 W kg⁻¹/750 mW cm⁻³), companied by remarkable cyclability (71% retention after 10 000 cycles), manifesting its great promise for large-scale integrated energy-storage system.     

The comparative influences of structural ordering, grain size, Li-content, and bulk density on the Li+-conductivity of Li0.29La0.57TiO3

The lattice and total Li⁺-ionic conductivity of Li_0.29La_0.57TiO₃ ceramic (LLTO) sintered at 1200 °C were determined as functions of powder calcination temperature and sintering duration, and these results were correlated with the relative degrees of Li⁺-ordering, Li-content, grain size, and bulk density to assess the relative impact of these parameters on material performance. Under all conditions, LLTO formed with a high degree of tetragonal superstructure to its perovskite related framework, and the lattice conductivity closely followed the relative amounts of the superstructure, as evaluated via determination of the sample ordering parameter from X-ray diffraction data. LLTO powders that were calcined at 900 °C for 1 h and sintered at 1200 °C for 6 h gave lattice conductivity values (~1.14 × 10⁻³ S cm⁻¹) comparable within the highest ranges reported in the literature. This coincided with the lowest degree of tetragonal superstructure formation, and it was also found to be largely independent of the values of Li-content measured on sintered ceramic despite significant Li₂O volatilization at longer sintering times (up to 23 % after 12 h at 1200 °C). Samples of LLTO powder that were calcined at 1100 °C and sintered at 1200 °C for 12 h resulted in the highest total Li-ion conductivity value ~6.30 × 10⁻⁵ S cm⁻¹. The total conductivity of LLTO varied inversely with grain size when the grains were <20 μm but was insensitive to that parameter above that size threshold. The strongest influence on total conductivity was primarily the bulk ceramic density. It was estimated from measured values that as the bulk ceramic density approached the full theoretical value for LLTO the total conductivity could near the lattice conductivity of ~1.2 × 10⁻³ S cm⁻¹.     

Hydrothermal synthesis of Fe3O4 nanoparticles and its application in lithium ion battery

Well dispersed Fe₃O₄ nanoparticles with a mean diameter of about 160 nm were synthesized by a simple hydrothermal method in the presence of sodium sulfate. The products were characterized by X-ray diffraction (XRD), field emission scanning electron microscopy (FE-SEM), transmission electron microscopy (TEM), Raman spectrum, and Fourier transform infrared spectra (FTIR). Electrochemical properties of the nanostructured Fe₃O₄ as cathode electrodes of lithium ion battery were studied by conventional charge/discharge tests, showing a high initial discharge capacity of 1267 mA h g^− 1 at a current density of 0.1 mA cm^− 2.     

Sandwich-Structured Quasi-Solid Polymer Electrolyte Enables High-Capacity,Long-Cycling,and Dendrite-Free Lithium Metal Battery at Room Temperature

The insufficient ionic conductivity, limited lithium-ion transference number (t_Li+), and high interfacial impedance severely hinder the practical application of quasi-solid polymer electrolytes (QSPEs). Here, a sandwich-structured polyacrylonitrile (PAN) based QSPE is constructedin which MXene-SiO₂ nanosheets act as a functional filler to facilitate the rapid transfer of lithium-ion in the QSPE, and a polymer and plastic crystalline electrolyte (PPCE) interface modification layer is coated on the surface of the PAN-based QSPE of 3 wt.% MXene-SiO₂ (SS-PPCE/PAN-3%) to reduce interfacial impedance. Consequently, the synthesized SS-PPCE/PAN-3% QSPE delivers a promising ionic conductivity of ≈1.7 mS cm⁻¹ at 30 °C, a satisfactory t_Li+ of 0.51, and a low interfacial impedance. As expected, the assembled Li symmetric battery with SS-PPCE/PAN-3% QSPE can stably cycle more than 1550 h at 0.2 mA cm⁻². The Li||LiFePO₄ quasi-solid-state lithium metal battery (QSSLMB) of this QSPE exhibits a high capacity retention of 81.5% after 300 cycles at 1.0 C and at RT. Even under the high-loading cathode (LiFePO₄ ≈ 10.0 mg cm⁻²) and RT, the QSSLMB achieves a superior area capacity and good cycling performance. Besides, the assembled high voltage Li||NMC811(loading ≈ 7.1 mg cm⁻²) QSSLMB has potential applications in high-energy fields.     

A High-Performance Hybrid Biofuel Cell with a Honeycomb-Like Ti3C2Tx/MWCNT/AuNP Bioanode and a ZnCo2@NCNT Cathode for Self-Powered Biosensing

This work focusses on developing a hybrid enzyme biofuel cell-based self-powered biosensor with appreciable stability and durability using murine leukemia fusion gene fragments (tDNA) as a model analyte. The cell consists of a Ti₃C₂T_x/multiwalled carbon nanotube/gold nanoparticle/glucose oxidase bioanode and a Zn/Co-modified carbon nanotube cathode. The bioanode uniquely exhibits strong electron transfer ability and a high surface area for the loading of 1.14 × 10⁻⁹ mol cm⁻² glucose oxidase to catalyze glucose oxidation. Meanwhile, the abiotic cathode with a high oxygen reduction reaction activity negates the use of conventional bioenzymes as catalysts, which aids in extending the stability and durability of the sensing system. The biosensor offers a 0.1 fm –1 nm linear range and a detection limit of 0.022 fm tDNA. Additionally, the biosensor demonstrates a reproducibility of ≈4.85% and retains ≈87.42% of the initial maximal power density after a 4-week storage at 4 °C, verifying a significantly improved long-term stability.     

Multiscale Structural Engineering of Sulfur/Carbon Cathodes Enables High Performance All-Solid-State Li?S Batteries

Constructing all-solid-state lithium–sulfur batteries (ASSLSBs) cathodes with efficient charge transport and mechanical flexibility is challenging but critical for the practical applications of ASSLSBs. Herein, a multiscale structural engineering of sulfur/carbon composites is reported, where ultrasmall sulfur nanocrystals are homogeneously anchored on the two sides of graphene layers with strong S C bonds (denoted as S@EG) in chunky expanded graphite particles via vapor deposition method. After mixing with Li_9.54Si_1.74P_1.44S_11.7Cl_0.3 (LSPSCL) solid electrolytes (SEs), the fabricated S@EG-LSPSCL cathode with interconnected “Bacon and cheese sandwich” feature can simultaneously enhance electrochemical reactivity, charge transport, and chemomechanical stability due to the synergistic atomic, nanoscopic and microscopic structural engineering. The assembled InLi/LSPSCL/S@EG-LSPSCL ASSLSBs demonstrate ultralong cycling stability over 2400 cycles with 100% capacity retention at 1 C, and a record-high areal capacity of 14.0 mAh cm⁻² at a record-breaking sulfur loading of 8.9 mg cm⁻² at room temperature as well as high capacities with capacity retentions of ≈100% after 600 cycles at 0 and 60 °C. Multiscale structural engineered sulfur/carbon cathode has great potential to enable high-performance ASSLSBs for energy storage applications.     

Heterointerface and Tensile Strain Effects Synergistically Enhances Overall Water-Splitting in Ru/RuO2 Aerogels

Designing robust electrocatalysts for water-splitting is essential for sustainable hydrogen generation, yet difficult to accomplish. In this study, a fast and facile two-step technique to synthesize Ru/RuO₂ aerogels for catalyzing overall water-splitting under alkaline conditions is reported. Benefiting from the synergistic combination of high porosity, heterointerface, and tensile strain effects, the Ru/RuO₂ aerogel exhibits low overpotential for oxygen evolution reaction (189 mV) and hydrogen evolution reaction (34 mV) at 10 mA cm⁻², surpassing RuO₂ (338 mV) and Pt/C (53 mV), respectively. Notably, when the Ru/RuO₂ aerogels are applied at the anode and cathode, the resultant water-splitting cell reflected a low potential of 1.47 V at 10 mA cm⁻², exceeding the commercial Pt/C||RuO₂ standard (1.63 V). X-ray adsorption spectroscopy and theoretical studies demonstrate that the heterointerface of Ru/RuO₂ optimizes charge redistribution, which reduces the energy barriers for hydrogen and oxygen intermediates, thereby enhancing oxygen and hydrogen evolution reaction kinetics.     

Effects of interstitial Li+ ions on the properties of novel Li4.08Zn0.04Si0.96O4 ceramic electrolyte

The aim of this work was to investigate the effects of interstitial ions in the novel Li_4 + 2xZn_xSi_1 − xO₄ (x = 0.04) compound prepared via sol gel method. The compound was indexed to the monoclinic unit cell in the space group P2_1/m and the chemical composition of the compound was very close to the designed composition. The introduction of two interstitial Li⁺ ions increased charge carrier concentration in the doped system resulting in an enhancement of conductivity by an order of magnitude as compared to that of the parent compound, Li₄SiO₄. The compound of Li_4.08Zn_0.04Si_0.96O₄ exhibited total conductivity values of 2.51 × 10^− 5 S cm^− 1 at ambient temperature and 3.01 × 10^− 3 S cm^− 1 at 500 °C. Ionic transference number corresponding to Li⁺ ion transport was also found to be higher than the value obtained for the parent compound. This proved that interstitial Li⁺ ions contributed to the total conductivity in the sample. Linear sweep voltammetry result showed that the Li_4.08Zn_0.04Si_0.96O₄ ceramic electrolyte was electrochemically stable up to 5.80 V versus a Li/Li⁺ reference electrode.     

High rate performance of novel cathode material Li1.33Ni1/3Co1/3Mn1/3O2 for lithium ion batteries

Li_1.33Ni_1/3Co_1/3Mn_1/3O₂ with highly ordered structure has been successfully synthesized via a simple co-precipitation process. Charge–discharge tests showed that the initial discharge capacities are 153.0 mAh g⁻¹ and 128.9 mAh g⁻¹ at 5 C (1000 mA g⁻¹) and 10 C (2000 mA g⁻¹) between 2.5 and 4.5 V, respectively. The average full-charge time of this material is less than 12 min at 5 C and 6 min at 10 C. The electrode material composed of the prepared showed a better cyclability. The excellent high rate performance is attributed to the improved ordered layered structure and the electrical conductivity. The excess Li shorten Li⁺ diffusion distance between these submicron and nano-scaled particles. The results show that Li_1.33Ni_1/3Co_1/3Mn_1/3O₂ cathode material has potential application in lithium ion batteries.     

Synergistically Accelerating Adsorption-Electrocataysis of Sulfur Species via Interfacial Built-In Electric Field of SnS2-MXene Mott–Schottky Heterojunction in Li-S Batteries

Developing efficient heterojunction electrocatalysts and uncovering their atomic-level interfacial mechanism in promoting sulfur-species adsorption-electrocatalysis are interesting yet challenging in lithium-sulfur batteries (LSBs). Here, multifunctional SnS₂-MXene Mott–Schottky heterojunctions with interfacial built-in electric field (BIEF) are developed, as a model to decipher their BIEF effect for accelerating synergistic adsorption-electrocatalysis of bidirectional sulfur conversion. Theoretical and experimental analysis confirm that because Ti atoms in MXene easily lost electrons, whereas S atoms in SnS₂ easily gain electrons, and under Mott–Schottky influence, SnS₂-MXene heterojunction forms the spontaneous BIEF, leading to the electronic flow from MXene to SnS₂, so SnS₂ surface easily bonds with more lithium polysulfides. Moreover, the hetero-interface quickly propels abundant Li⁺/electron transfer, so greatly lowering Li₂S nucleation/decomposition barrier, promoting bidirectional sulfur conversion. Therefore, S/SnS₂-MXene cathode displays a high reversible capacity (1,188.5 mAh g⁻¹ at 0.2 C) and a stable long-life span with 500 cycles (≈82.7% retention at 1.0 C). Importantly, the thick sulfur cathode (sulfur loading: 8.0 mg cm⁻²) presents a large areal capacity of 7.35 mAh cm⁻² at lean electrolyte of 5.0 µL mg_s⁻¹. This work verifies the substantive mechanism that how BIEF optimizes the catalytic performance of heterojunctions and provides an effective strategy for deigning efficient bidirectional Li-S catalysts in LSBs.     

Chemical diffusion coefficient of lithium ion in Li3V2(PO4)3 cathode material

The kinetic properties of monoclinic lithium vanadium phosphate were investigated by potential step chronoamperometry (PSCA) and electrochemical impedance spectroscopy (EIS) method. The PSCA results show that there exists a linear relationship between the current and the square root of the time. The D?_Li values of lithium ion in Li_3-xV₂(PO₄)₃ under various initial potentials of 3.41, 3.67, 3.91 and 4.07 V (vs Li/Li⁺) obtained from PSCA are 1.26 × 10^− 9, 2.38 × 10^− 9, 2.27 × 10^− 9 and 2.22 × 10^− 9 cm²·s^− 1, respectively. Over the measuring temperature range 15-65 °C, the diffusion coefficient increased from 2.67 × 10^− 8 cm²·s^− 1 (at 15 °C) to 1.80 × 10^− 7 cm²·s^− 1 (at 65 °C) as the measuring temperature increased.     

Sodium Stoichiometry Tuning of the Biphasic-NaxMnO2 Cathode for High-Performance Sodium-Ion Batteries

Sodium-ion batteries (SIBs) are promising alternatives for large-scale energy storage owing to the rich resource and cost effectiveness. However, there are limitations of suitable low-cost, high-rate cathode materials for fast charging and high-power delivery in grid systems. Herein, a biphasic tunnel/layered 0.80Na_0.44MnO₂/0.20Na_0.70MnO₂ (80T/20L) cathode delivering exceptional rate performance through subtly regulating the sodium and manganese stoichiometry is reported. It delivers a reversible capacity of 87 mAh g⁻¹ at 4 A g⁻¹ (33 C), much higher than that of tunnel Na_0.44MnO₂ (72 mAh g⁻¹) and layered Na_0.70MnO₂ (36 mAh g⁻¹). It proves that the one-pot synthesized 80T/20L is able to suppress the deactivation of L-Na_0.70MnO₂ under air-exposure, which improves the specific capacity and cycling stability. Based on electrochemical kinetics analysis, the electrochemical storage of 80T/20L is mainly based on pseudocapacitive surface-controlled process. The thick film of 80T/20L cathode (a single-side mass loading over 10 mg cm⁻²) also has superior properties of pseudocapacitive response (over 83.5% at a low sweep rate of 1 mV s⁻¹) and excellent rate performance. In this sense, the 80T/20L cathode with outstanding comprehensive performance could meet the requirements of high-performance SIBs.     

P and Se Binary Vacancies and Heterostructures Modulated MoP/MoSe2 Electrocatalysts for Improving Hydrogen Evolution and Coupling Electricity Generation

It is not enough to develop an ideal hydrogen evolution reaction (HER) electrocatalysts by single strategy. Here, the HER performances are significantly improved by the combined strategies of P and Se binary vacancies and heterostructure engineering, which is rarely explored and remain unclear. As a result, the overpotentials of MoP/MoSe₂-H heterostructures rich in P and Se binary vacancies are 47 and 110 mV at 10 mA cm⁻² in 1 m KOH and 0.5 m H₂SO₄ electrolytes, respectively. Especially, in 1 m KOH, the overpotential of MoP/MoSe₂-H is very close to commercial Pt/C at the beginning and even better than Pt/C when current density is over 70 mA cm⁻². The strong interactions between MoSe₂ and MoP facilitate electrons transfer from P to Se. Thus, MoP/MoSe₂-H possesses more electrochemically active sites and faster charge transfer capability, which are all in favor of high HER activities. Additionally, Zn-H₂O battery with MoP/MoSe₂-H as cathode is fabricated for simultaneous generation of hydrogen and electricity, which displays the maximum power density of up to 28.1 mW cm⁻² and stable discharging performance for 125 h. Overall, this work validates a vigorous strategy and provides guidance for the development of efficient HER electrocatalysts.