Three-dimensional Porous Framework Research Articles

In situ anchoring of MnO nanoparticles into three-dimensional nitrogen-doped porous carbon framework as a stable anode for high-performance lithium storage

Although transition metal oxides have the advantages of large theoretical capacity, low cost and eco-friendliness, their application as anodes for lithium-ion batteries (LIBs) is still limited due to their undesirable electrical conductivity and large volume expansion. Herein, a novel two-step rapid freeze-drying-calcination strategy was applied to prepare highly dispersed nano-MnO-anchored three-dimensional nitrogen-doped porous carbon framework composites (MnO@3D N-PCF). Compared with MnO and undoped MnO@3D PCF, the MnO@3D N-PCF anode exhibits superb cycle stability, remarkable specific capacity and impressive high-rate performance (1037.0 mAh g−1 over 100 cycles at 0.1 A g−1 and 760.9 mAh g−1 over 500 cycles at 5 A g−1), mainly due to its well-designed 3D nanoarchitecture. It is found that 3D nitrogen-doped carbon networks can act as stable conductive bridges to facilitate electron transport and sufficient diffusion channels for Li ions. The MnO nanoparticles obtained by rapid lyophilization and calcination technology are highly dispersed in the porous 3D carbon skeleton, which can buffer volume expansion and preserve the stability of the electrode. It is expected that this simple and green synthesis strategy will open the door for the development of transition metal oxide/carbon three-dimensional nanocomposites with high stability and excellent electrochemical properties.

A 3D porous framework constructed from [(PIIIO3)2Mo5O15]6− clusters and {Cu(en)2} units: Synthesis, crystal structure and electrochemical properties

A new organic-inorganic hybrid, formulated as the H2[Cu(en)2]2[(PIIIO3)2Mo5O15]·4H2O (denoted as CuenP2Mo5) (en=ethylenediamine), was isolated via in situ self-assembly reaction of H3PO3, (NH4)6Mo7O24.4H2O, en, and CuCl2·2H2O in the aqueous solution. Structural analysis reveals that CuenP2Mo5 display a three-dimensional (3D) porous framework assembled from the [(PIIIO3)2Mo5O15]6− clusters linked with the {Cu(en)2} units. The morphology of CuenP2Mo5 feature a lamellar construction, smooth surface and regular edges with sizes 50–100 µm. Electrochemical studies reveal that CuenP2Mo5 exhibits the multi-electron redox processes ascribed to MoVI and CuII centers, and has good electrocatalytic activity in the reduction of H2O2. CuenP2Mo5 modified electrode shows a wide linear range (50–450 µM), high sensitivity of 1.76 µA·µM−1 and a low detection limit of 0.45 µM for the electrochemical detection of H2O2.

Synthesis and Structure of a Copper-Based Functional Network for Efficient Organic Dye Adsorption.

In the work, by incorporating polyoxometalates (POMs) into a copper(II)-based network, a novel three-dimensional (3D) porous framework, [Cu17Cl3(trz)12]H3[GaW12O40]·9H2O (Cu-GaW-TRZ), was successfully prepared and explored for the adsorption of dyes. The adsorption capacity of Cu-GaW-TRZ was calculated as 13.11 mg/g, and the dye adsorption rate equaled 96.2% for the adsorption of methylene blue (MB). Furthermore, this recyclable adsorbent is stable enough without obvious loss of adsorption capacity for at least five runs. Meanwhile, the structure of the macropores is suitable for the entry of large molecular dyes, and [GaW12O40]5- also can achieve efficient adsorption for cationic dyes. The results displayed a pseudo-second-order kinetic model and were well matched for MB adsorption onto Cu-GaW-TRZ. The free energy, entropy, and enthalpy of the thermodynamic parameters for the adsorption of MB were calculated, which revealed that the adsorption process was befitting for the adsorption of MB.

High-Symmetry Co/Ni Triazine Polycarboxylate Diverse Frameworks Constructed by Mx(COO)y Building Blocks: Characterization and Catalytic Performance Evaluation of p-Nitrophenol.

Three new triazine compounds [Co1.5(H3TDPAT)(H2O)3]·6H2O (1), [Co2(TCPT)(μ2-H2O)2]·OH (2), and [Ni3(TCPT)]·3OH (3) were designed and synthesized via the reaction of the symmetrical triazine ligand connected by C-N-C and C-O-C bonds with triazine poly(carboxylic acid)s ligands as the side arms: H6TDPAT (H6TDPAT = 2,4,6-tris(3,5-dicarboxylphenylamino)-1,3,5-triazine) and H3TCPT (H3TCPT = 2,4,6-tris(4-carboxyphenoxy)-1,3,5-triazine) as well as the corresponding metal salts under the solvothermal condition. Three triazine polycarboxylate frameworks were characterized by elemental analysis, infrared spectroscopy, ultraviolet spectroscopy, thermogravimetric analysis, X-ray powder diffraction, and solid fluorescent spectra in detail. The structural analysis results showed that the three-dimensional porous cage framework of compound 1 was constructed by three different polyhedral cages connected with [Co(COO)4(H2O)2] building blocks. One of the compounds, 2, is formed by twin propeller Co2(μ2-H2O)(COO)3 building blocks connecting two-dimensional layers and the intermolecular π-π interactions involved the triazine rings between the layers. While the structure of compound 3 is similar to that of 2, assembly is by Ni(COO)3 building blocks and adjacent layers of the face-to-face π-π interaction between the triazine rings. In order to explore functional properties, the catalytic reduction of p-nitrophenol (PNP) of compounds 1-3 was investigated. They exhibit excellent catalytic activity of more than 95% for reduction of PNP with a dose of 2.5 mg of the compounds.

Adamantane Three-Dimensional Porous Organic Framework as a Fluorescence Sensor for Rapid Determination of Tetracycline in Aquatic Products

A fluorescence adamantane three-dimensional porous organic framework (AdaPOF) was synthesized via a Suzuki coupling reaction. The AdaPOF showed excellent fluorescence performance with a relative high quantum yield and fluorescence stability. Due to its excellent selectivity to tetracycline (TC), a fluorescence sensor based on AdaPOF was constructed for TC determination. The selective sensing mechanism of the AdaPOF towards TC was studied by density functional theory (DFT) calculation experiments. An AdaPOF–based fluorescence method for TC determination was established, with the linear range of 0.1–9.0 μmol/L (R2 = 0.9959) and the limit of detection (S/N = 3) of 43 nmol/L. Moreover, the fluorescence method was used to the determination of TC in aquatic products and the recoveries were ranged from 94.4% to 103.8%. The results obtained by this fluorescence method were consistent with those of the high-performance liquid chromatography (HPLC) method in the TC determination.

Constructing 3D Tent-Like frameworks in melamine hybrid foam for superior microwave absorption and thermal insulation

Taking serious electromagnetic pollution and practical application requirements into consideration, it’s imperative to develop multifunctional microwave absorption materials. In this work, the phenol–formaldehyde resin (PF) successfully adheres to melamine–formaldehyde foam (MF) as three-dimensional (3D) porous frameworks, and subsequently the substrate anchors few-layered MXene nanosheets by dripping-squeeze-drying procedures. According to the results, the hollow tent-like structure of MXene/PF@MF (MPM) shows a significant effect on microwave absorption capability, including extending heterogeneous interfaces for polarization relaxation and prolonging microwave propagation paths for energy dissipation. Based on the synergy of multiple components and rational structure, MPM exhibits a minimum reflection loss (RLmin) value of −58.8 dB at 2.2 mm and achieves an effective absorption bandwidth (EAB) of 6.74 GHz covering the entire Ku band. The microwave absorption mechanism reveals that the superior microwave absorption capability results from high conduction loss, polarization relaxation, multiple attenuations, and appropriate impedance matching. Furthermore, the MPMs possess lightweight features (32.7–48.7 g cm−3) and low thermal conductivity (0.0309–0.0318 W m−1 K−1) benefitting the unique 3D porous structure. Meanwhile, the low thermal conductivity endows MPMs with infrared stealth, which broadens the application in military fields. This work proposes a facile strategy for constructing highly efficient microwave absorbers with multiple functions.

Tetraethyl orthosilicate steam induced silicon-based anticorrosion film enables highly reversible zinc metal anodes for zinc-iodine batteries

Zinc (Zn) metal anodes are badly troubled by the challenges of notorious dendrites and corrosion reactions from H2O and I3− ions during stripping/plating processes, impeding the commercial application of Zn-iodine (I2) batteries. In this work, we report a novel strategy for the in-situ construction of uniform silicon-based anticorrosion films on Zn metal anodes (Zn@Ts) through the treatment of tetraethyl orthosilicate (TEOS) steam on Zn disks for different times. TEOS can be decomposed into three-dimensional (3D) porous inorganic frameworks (SiOxCy) filled with organic polymers (SiCxOyHz) on Zn metal at 180 °C in autoclave. On the one hand, silicon-based composite layers can protect Zn metal from direct contact with aqueous electrolyte and stabilize the electrode/electrolyte interface, which hinders the occurrence of hydrogen evolution as well as corrosion reactions. On the other hand, 3D macroporous structure not only provides strong mechanical framework but also guides Zn2+ flux to homogenize Zn2+ concentration and realize uniform Zn nucleation/deposition, which contributes to suppress the growth of Zn dendrites. Zn@Ts symmetric batteries exhibit better cycling life of 5000 h comparing with bare Zn at 2 mA cm−2 and 2 mA h cm−2. Zn–I2 full-cells can achieve 89 mA h g−1 and 93% capacity retention after 20000 cycles.

Flux crystal growth of rubidium–iron silicates and germanates and their ion-exchange using alkali nitrate salts

Single crystals of two new rubidium ferrites, RbFeSiO4 and RbFeGeO4, were grown out of a eutectic RbCl–RbF melt. Both compounds crystallize in the noncentrosymmetric orthorhombic space group Ima2 and exhibit a three-dimensional porous framework structure composed of statistically disordered (Fe/T)O4 (T = Si, Ge) tetrahedra that corner-share to generate large channels running down the c-axis. These channels are occupied by Rb ions to maintain charge balance. RbFeSiO4 can also be prepared via a solid-state reaction by mixing and heating stoichiometric amounts of Rb2CO3, Fe2O3 and elemental Si; however, a similar approach for preparing RbFeGeO4 yielded a mixture of RbFeGeO4 and RbFeGe2O6. Powder second harmonic generation (SHG) measurements of RbFeSiO4 determined that the material is SHG-active with an intensity of 0.5 times of α-SiO2. First principles calculations in the form of density-functional theory indicated that it would be possible to ion exchange the Rb cation for other alkali metal cations. Applying a molten alkali nitrate salt-bath treatment at low soak temperatures of 350 °C–450 °C and short soak times of ∼16 h resulted in the almost complete replacement of rubidium with potassium and the partial replacement of rubidium with cesium, yielding K0.92Rb0.08FeSiO4, K0.91Rb0.09FeGeO4, and Cs0.48Rb0.52FeGeO4. No ion-exchange was observed when RbFeSiO4 was soaked in molten CsNO3; however, it was possible to force the exchange by using a CsCl melt at 680 °C to yield Cs0.13Rb0.87FeSiO4.

Self-powered air purifier with coupling of non-thermal plasma and photocatalytic oxidation for formaldehyde degradation based on triboelectric nanogenerator

The emission of various volatile organic compounds (VOCs) caused by indoor decoration and furniture placement are the causes of health hazards in people's lives. Here, we demonstrate a self-powered air purifier for indoor organic pollutant removal based on triboelectric nanogenerator (TENG), coupling non-thermal plasma (NTP) with photocatalytic oxidation (PCO). An adjustable external high voltage field is generated by our homemade TENG, in which the output open-circuit voltage (Voc) ranges from 10 to 30 kV. After connecting the TENG with a non-thermal plasma generator (NTP-G), a maximum ozone concentration of 14.7 mg/m³ and NTP can be generated. The prepared three-dimensional porous framework is used as a photocatalytic layer, which can support more titanium oxide and increase the contact area between the photocatalyst and formaldehyde. This designed self-powered air purifier can reduce the formaldehyde concentration from 2.06 ppm to 0 ppm in 21 min in a 13 L closed air chamber. The design and concept proposed in this work has multiple ways for formaldehyde degradation and are not limited by sunlight, and can remove indoor formaldehyde around the clock, providing an effective way to create a cleaner and healthier indoor environment.

New insights into the outstanding performances of nickel‐doped manganese oxide nanoparticles embedded in a 3D carbon nanopipes framework as anode for lithium and sodium‐ion batteries

A new nanocomposite system based on Ni-doped Mn3O4 nanoparticles embedded in three-dimensional porous carbon nanopipes framework CMK-5 is developed by combination of repeat templating and wet-impregnation techniques to evaluate its performances as anode for rechargeable batteries. The nanocomposite materials are synthesized by varying the Mn3O4 and nickel amounts. Among the nanocomposites, the Ni(5)-Mn3O4(1)@CMK-5 anode exhibits outstanding discharge capacity of 1269 mA h g−1 after 200 cycles and 832 mA h g−1 beyond 500 cycles at 100 and 1000 mA g−1, respectively, for lithium-ion batteries (LIBs). Even at high current of 2000 mA g−1, the electrode possesses the capacity of 669 mA h g−1. When the Ni(5)-Mn3O4(1)@CMK-5 anode is used in sodium-ion batteries (SIBs), it provides remarkable discharge capacities of 490 and 334 mA h g−1 after 500 cycles at 50 and 100 mA g−1, respectively. The excellent electrochemical performances of the Ni(5)-Mn3O4(1)@CMK-5 nanocomposite reveal its promising potentials as anode for LIBs and SIBs.

A Three-Dimensional Melamine Sponge Modified with MnOx Mixed Graphitic Carbon Nitride for Photothermal Catalysis of Formaldehyde.

Much attention has been paid to developing effective visible light catalytic technologies for VOC oxidation without requiring extra energy. In this paper, a series of sponge-based catalysts with rich three-dimensional porosity are synthesized by combining MnOx and graphitic carbon nitride (GCN) with commercial melamine sponges (MS) coated with polydopamine (PDA), demonstrating excellent photothermal catalytic performance for formaldehyde (HCHO). The three-dimensional porous framework of MS can provide a good surface for material modification and a reliable interface for gas-solid interaction. The grown layer of PDA framework not only increases the near-infrared wavelength absorption for improving the light-to-heat conversion of catalysts, but also brings excellent adhesion for the subsequent addition of MnOX and GCN. The efficient formaldehyde oxidation is attributed to the sufficient oxygen vacancies generated by co-loaded MnOX and GCN, which is conducive to the activation of more O2− in the oxidation process. As the surface temperature of catalyst rapidly increases to its maximum value at ca. 115 °C under visible light irradiation, the HCHO concentration drops from 160 ppm to 46 ppm within 20 min. The reaction mechanism is certified as a classical Mars-van Krevelen mechanism based on the photo-induced thermal catalysis process.

Three-dimensional porous framework constructed by hybrid of carbon nanotubes and carbon nanocoils for stable lithium metal anode

Three-dimensional porous framework constructed by hybrid of carbon nanotubes and carbon nanocoils for stable lithium metal anode

Mechanically Interlocked Aerogels with Densely Rotaxanated Backbones.

Mechanically interlocked molecules are considered promising candidates for the construction of self-adaptive materials by virtue of their fascinating structural and dynamic features. However, it is still a great challenge to fabricate such materials with higher complexity and richer functionality. Herein, we propose the concept of mechanically interlocked aerogels (MIAs) in which the three-dimensional (3D) porous frameworks are made of dense mechanically interlocked modules, thereby enabling the integration of mechanical adaptivity and multifunctionality in a single entity. The lightweight MIA monoliths possess a good appearance and hierarchical meso- and submicron-pores. Profiting from the combination of dynamic mechanical bonds and porous skeletons of aerogels, our MIAs are not only mechanically robust (average Young's modulus = 5.80 GPa and specific modulus = 130.5 kN·m/kg) but also showcase favorable mechanical adaptivity and responsiveness under external stimuli. Taking advantage of the above integrative merits, we demonstrate the multifunctionality of our MIAs in terms of iodine uptake, thermal insulation, and selective adsorption of organic dyes. Our work opens the door to designing intelligent aerogels with delicate topological chemical structures while facilitating the development of mechanically interlocked materials.

Detachable all-carbon-linked 3D covalent organic framework films for semiconductor/COF heterojunctions by continuous flow synthesis

Detachable all-carbon-linked 3D covalent organic framework films for semiconductor/COF heterojunctions by continuous flow synthesis

The Scalable Solid-State Synthesis of a Ni5P4/Ni2P-FeNi Alloy Encapsulated into a Hierarchical Porous Carbon Framework for Efficient Oxygen Evolution Reactions.

The exploration of high-performance and low-cost electrocatalysts towards the oxygen evolution reaction (OER) is essential for large-scale water/seawater splitting. Herein, we develop a strategy involving the in situ generation of a template and pore-former to encapsulate a Ni5P4/Ni2P heterojunction and dispersive FeNi alloy hybrid particles into a three-dimensional hierarchical porous graphitic carbon framework (labeled as Ni5P4/Ni2P–FeNi@C) via a room-temperature solid-state grinding and sodium-carbonate-assisted pyrolysis method. The synergistic effect of the components and the architecture provides a large surface area with a sufficient number of active sites and a hierarchical porous pathway for efficient electron transfer and mass diffusion. Furthermore, a graphitic carbon coating layer restrains the corrosion of alloy particles to boost the long-term durability of the catalyst. Consequently, the Ni5P4/Ni2P–FeNi@C catalyst exhibits extraordinary OER activity with a low overpotential of 242 mV (10 mA cm−2), outperforming the commercial RuO2 catalyst in 1 M KOH. Meanwhile, a scale-up of the Ni5P4/Ni2P–FeNi@C catalyst created by a ball-milling method displays a similar level of activity to the above grinding method. In 1 M KOH + seawater electrolyte, Ni5P4/Ni2P–FeNi@C also displays excellent stability; it can continuously operate for 160 h with a negligible potential increase of 2 mV. This work may provide a new avenue for facile mass production of an efficient electrocatalyst for water/seawater splitting and diverse other applications.

Rationally designed In@Zn@In trilayer structure on 3D porous Cu towards high-performance Zn-Ion batteries

Metallic Zn has been regarded as a promising anode for rechargeable aqueous zinc-ion batteries (ZIBs) due to its abundant reserves, low cost, high safety, low redox potential and high theoretical capacity. However, such ZIBs usually suffer from dendrite growth and serious side reactions of Zn anode, and incur poor cycling stability and battery safety issues, thus limiting their practical applications. Herein a unique In@Zn@In trilayer structure grown on three-dimensional (3D) porous Cu framework (3D In@Zn@In) is rationally designed and developed by electroless plating coupled with electrodepositing for high-performance ZIBs. The sandwich-like In@Zn@In trilayer structure not only efficiently inhibits the dendrite growth and side reactions of Zn anode, but also exhibits remarkably enhanced Zn plating/stripping kinetics. Meanwhile, 3D porous architectures possess some favorable merits for ZIBs including rapid electrolyte penetration, sufficient electron/ion transport channels, restricting Zn dendrite growth, and robust structure integrity. In this work, 3D In@Zn@In efficiently combines the advantages of In@Zn@In trilayer structure and 3D porous framework, and shows highly stable Zn storage for over 400 h in symmetry cell and 2000 cycles in full cell coupled with Mn2O3 cathode. This work provides a facile, efficient and controllable strategy to inhibit Zn dendrite and side reactions for realizing highly stable Zn anode, showing a great potential for other metal anode applications.

Methyl orange-crosslinked polypyrrole hydrogel enabled N, O, S co-doped porous carbon for highly sensitive determination of three redox-active biomolecules

• A nanostructured PPy hydrogel is designed for the first time with methyl orange as crosslinker. • The methyl orange crosslinked PPy hydrogel enables N, O, S co-doped three-dimensional porous carbon frameworks (N, O, S-HCF). • N, O, S-HCF delivers an outstanding electroanalytical activity and selectivity for the simultaneous determination of three redox-active biomolecules. Development of a high-performance electrode materials for the simultaneous sensing of ascorbic acid (AA), dopamine (DA) and uric acid (UA) is critical in clinical diagnostics. Novel polymer hydrogel-derived porous carbon has been investigated in sensing due to their high conductivity, hierarchical porous structure and environmental benignity. However, the high cost and cumbersome synthesis of the crosslinker for polymer hydrogel precursors make carbon production by pyrolysis greatly compromised. To address this challenge, here, a facile approach to N, O, S co-doped three-dimensional porous carbon frameworks (N, O, S-HCF) derived from methyl orange (MO) crosslinked polypyrrole hydrogel is developed. Experimental and spectroscopy demonstrate that the derived 3D porous structure and heteroatom doping effect create multidimensional electron transfer pathways and electrocatalytic activity centers. Specifically, the sensor exhibits potent and persistent electrochemical behavior with well-separated oxidation peaks and enhanced oxidation peak currents towards ascorbic acid (AA), dopamine (DA) and uric acid (UA). As a result, the N, O, S-HCF contributes to the effective determination of the three analytes in their mixture and the calibration curves show linear range of 2.5 × 10 −6 –1.0 × 10 −2 M, 1.8 × 10 −7 –8.7 × 10 −5 M, and 2.5 × 10 −7 –1.0 × 10 −4 M with detection limits of 1.0 × 10 −6 , 1.2 × 10 −7 , and 1.8 × 10 −7 M for AA, DA and UA, respectively. This study provides a simple strategy to build heteroatom doped porous carbon for the simultaneous monitoring of multiple electroactive species.

A lithiophilic hyperbranched polymer-decorated three-dimensional carbon skeleton boosting highly reversible lithium metal anode

The short cycling lifespan and serious safety issues caused by the crazy growth of dendrites, have severely restricted the practical application of Li metal anodes (LMAs) in high energy density batteries. Here, a three-dimensional (3D) porous conductive framework enriched with lithiophilic functional groups is proposed for stabilizing Li metal anodes, which is fabricated by coating hyperbranched polyol (HP) on the carbon fiber cloth (CFC) through a simple esterification reaction. The abundant lithiophilic groups distributed on HP can disperse the Li ion flow and guide the uniform nucleation of Li. The 3D porous skeleton not only promotes ion diffusion and electron transport but also provides adequate space for Li storage. Symmetrical battery configurated with CFC@HP-Li hybrid anode demonstrates stable cycling over 800 h with low voltage hysteresis at a current density of 2 mA cm−2. With a commercial LiFePO4 (LFP) cathode, the CFC@HP-Li//LFP full battery can realize a high capacity retention rate of 88.9% and a stable Coulombic efficiency (CE) close to 100% after 500 cycles at 2 C. The CFC@HP-Li anode, which is constructed by a modification of LMAs using the targeted lithiophilic coating, provides a promising strategy for the exploration of high-performance Li metal batteries (LMBs).

Kinetically boosted potassium ion storage capability of 1D K2Ti6O13 nanobelts by 3D porous carbon framework for fiber-shaped potassium ion capacitors

One dimensional (1D) fiber-shaped energy storage device demonstrates a great potential for the future power source textiles. However, delivering high energy/power densities and long cycle life is still the crucially electrochemical themes to meet the ever-stringent demands. Herein, we report a novel non-aqueous fiber-shaped potassium ion capacitors (PICs), in which 1D K2Ti6O13 nanobelts (KTO) interweaved with three-dimensional (3D) porous carbon framework was synthesized as anode materials. The low specific capacity and sluggish reaction kinetics of the bare KTO is boosted by the 3D porous carbon framework. Its hierarchical porosity and 3D structure impede the aggregation of the KTO, and favor the permeation of potassium ions in electrolyte. Its graphitic carbon improves the electrical conductivity of the KTO. Meanwhile, it also offers a suitable potassium ion storage capacity. These features enable KTO@3D-C with high specific capacity and rate performance. A single non-aqueous fiber-shaped PICs with a high working voltage up to 3.5 V can lead to maximum areal and volumetric energy densities of 12.1 μWh cm−2 and 1.9 m Wh cm−3, indicating apparent energy advantages over the ones with aqueous electrolyte and symmetric configuration. Our integratable and robust fiber-shaped PICs prototype demonstrates a great potential for future power source textiles.

Three-Dimensional Porous Carbon/Nitrogen Framework-Decorated Palladium Nanoparticles for Stable and Wide-Concentration-Range Hydrogen Sensing.

Hydrogen (H2) as a high-energy-density carrier is of great potential in the upcoming hydrogen economy. Nevertheless, H2/air mixtures are explosive at H2 concentrations above 4 v/v % and reliable and wide-concentration-range H2 sensors are thus highly desired. Here, hydrogen sensing has been developed using palladium nanoparticles of ∼11.2 nm in diameter chemically decorated on the carbon/nitrogen three-dimensional porous framework of 308 m2 g-1 in specific surface area (Pd NPs@CN 3D framework). Theoretically, the Pd NPs and CN 3D framework are used to construct the Mott-Schottky heterojunctions, in which the CN 3D framework possesses a higher work function, promoting electron transfer to Pd NPs and therefore highly active dissociation of H2. Beneficially, the Pd NPs@CN 3D framework exhibits a wide concentration range of 200 ppm (S ≈ 0.2% and Tres ≈ 15 s) to 40 v/v % (S ≈ 73.8% and Tres ≈ 9 s) H2 sensing at room temperature. Remarkably, the H2 sensor prototype built with the Pd NPs@CN 3D framework shows excellent long-term stability that maintains reliable H2 sensing after 142 days. Such stable hydrogen sensing provides an experimental basis for the wide-concentration-range detection of H2 leakage in the future hydrogen economy.