Famatinite (Cu₃SbS₄, p-type) and chalcopyrite (CuFeS₂, n-type) are well-recognized sustainable minerals with good intermediate-temperature thermoelectric performance. In this article, we utilize the inherent thermoelectric properties of these compounds to demonstrate real-time operational performance as a coupled thermoelectric generator (TEG) for waste heat recovery applications. First, we synthesized the polycrystalline and nano-grained famatinite and chalcopyrite materials with high purity through a sustainable synthesis process of mechanical alloying followed by hot pressing. A maximum output power of ~5 mW by the developed TEG was demonstrated while harvesting from a waste heat source of 723 K. Furthermore, the TEG performance via computational simulations for varied thermal gradients was validated. Our results highlight the sustainable development of thermoelectric power generator from earth-abundant minerals having strong stability and capacity to convert waste heat to electricity, which opens a new direction for fabricating a low-cost TEG for intermediate-temperature applications.

Ruthenium (Ru)-based electrocatalysts show great promise as substitutes for platinum (Pt) for the alkaline hydrogen evolution reaction (HER) because of their efficient water dissociation capabilities. Nevertheless, the strong adsorption of Ru–OH intermediates (Ru-OH_ad) blocks the active site, leading to unsatisfactory HER performance. In this study, we report a universal ligand-exchange strategy for synthesizing a MOF-on-MOF-derived FeP–CoP heterostructure-anchored Ru single-atom site catalyst (Ru-FeP-CoP/NPC). The obtained catalyst shows a low overpotential (28 mV at 10 mA cm⁻²) and a high mass activity (9.29 A mg⁻¹ at 100 mV), surpassing the performance of commercial Pt/C by a factor of 46. Theoretical studies show that regulating the local charge distribution of Ru single-atom sites could alleviate surrounding OH⁻ blockages, accelerating water dissociation and facilitating hydrogen adsorption/desorption, thus enhancing HER activity. This work aims to inspire further design of highly active and durable electrocatalysts with tailored electronic properties for high-purity hydrogen production.

Currently, although some progress has been made in infancy-stage rocking-chair aqueous zinc-ion batteries (AZIBs), more discussions have focused only on the different electrochemical performances displayed by different material types rather than the intrinsic ion transport migration electrochemistry. Herein, we for the first time delve into the mechanism of tailoring the solvation sheath and desolvation processes at the electrode/electrolyte interfaces to enhance the structural stabilities in the deep discharge states. In this work, the TiO₂ front interfaces are induced on electrochemically active but unstable TiSe₂ host materials to construct unique TiO₂/TiSe₂–C heterointerfaces. According to X-ray absorption near edge structure (XANES), differential electrochemical mass spectrometry (DEMS), and electrochemical quartz crystal microbalance (EQCM), the intercalated species are transformed from [Zn(H₂O)₆]²⁺ to [Zn(H₂O)₂]²⁺ due to the built-in electric fields (BEFs) effects, further accelerating the ion transfer kinetics. Furthermore, owing to the absence of high-energy desolvation solvents released from desolvation processes, hydrogen evolution reaction (HER) energy barriers, Ti–Se bond strength, and structural stabilities are significantly improved, and the initial CE and HER overpotentials of the TiO₂/TiSe₂–C heterointerfaces increased from 13.76% to 84.7%, and from 1.04 to 1.30 V, respectively, and the H₂ precipitation current density even at −1.3 V decreased by 73.2%. This work provides valuable insights into the complex interface electrochemical mechanism of tailoring the solvation sheath and desolvation processes toward rocking-chair zinc-ion batteries.

Lithium–carbon dioxide (Li–CO₂) batteries with high theoretical energy density are regarded as promising energy storage system toward carbon neutrality. However, bidirectional catalysts design for improving the sluggish CO₂ reduction reaction (CO₂RR)/CO₂ evolution reaction (CO₂ER) kinetics remains a huge challenge. In this work, an advanced catalyst with fast-interfacial charge transfer was subtly synthesized through element segregation, which significantly improves the electrocatalytic activity for both CO₂RR and CO₂ER. Theoretical calculations and characterization analysis demonstrate local charge redistribution at the constructed interface, which leads to optimized binding affinity towards reactants and preferred Li₂CO₃ decomposition behavior, enabling excellent catalytic activity during CO₂ redox. Benefiting from the enhanced charge transfer ability, the designed highly efficient catalyst with dual active centers and large exposed catalytic area can maintain an ultra-small voltage gap of 0.33 V and high energy efficiency of 90.2%. This work provides an attractive strategy to construct robust catalysts by interface engineering, which could inspire further design of superior bidirectional catalysts for Li–CO₂ batteries.

By the random distribution of metals in a single phase, entropy engineering is applied to construct dense neighboring active centers with diverse electronic and geometric structures, realizing the continuous optimization of multiple primary reactions for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). Many catalysts developed through entropy engineering have been built in nearly equimolar ratios to pursue high entropy, hindering the identification of the active sites and potentially diluting the concentration of real active sites while weakening their electronic interactions with reaction intermediates. Herein, this work proposes an entropy-engineering strategy in metal nanoparticle-embedded nitrogen carbon electrocatalysts, implemented by entropy-engineered Prussian blue analogs (PBA) as precursors to enhance the catalytic activity of primary Cu-Fe active sites. Through the introduction of the micro-strains driven by entropy engineering, density functional theory (DFT) calculations and geometric phase analysis (GPA) using Lorentz electron microscopy further elucidate the optimization of the adsorption/desorption of intermediates. Furthermore, the multi-dimensional morphology and the size diminishment of the nanocrystals serve to expand the electrochemical area, maximizing the catalytic activity for both ORR and OER. Notably, the Zn-air battery assembled with CuFeCoNiZn-NC operated for over 1300 h with negligible decay. This work presents a paradigm for the design of low-cost electrocatalysts with entropy engineering for multi-step reactions.

Regulating the freedom and distribution of H₂O molecules has become the decisive factor in enlarging the electrochemical stability window (ESW) of aqueous electrolytes. Compared with the water in a bulk electrolyte, H₂O molecules at the electrode–electrolyte interface tend to directly split under bias potential. Therefore, the composition and properties of the interfacial microenvironment are the crux for optimizing ESW. Herein, we developed a heterogel electrolyte with wide ESW (4.88 V) and satisfactory ionic conductivity (4.4 mS/cm) inspired by the bicontinuous architecture and surfactant self-assembly behavior in the ionic liquid microemulsion-based template. This electrolyte was capable of expanding the ESW through the dynamic oil/water/electrode interface ternary structure, which enriched the oil phase and assembled the hydrophobic surfactant tails at the interface to prevent H₂O molecules from approaching the electrode surface. Moreover, the surfactant Tween 20 and polymer network effectively suppressed the activity of H₂O molecules through H-bond interactions, which was beneficial in expanding the operating voltage range and improving the temperature tolerance. The prepared gel electrolyte demonstrated unparalleled adaptability in various aqueous lithium-based energy storage devices. Notably, the lithium-ion capacitor showed an extended operating voltage of 2.2 V and could provide a high power density of 1350.36 W/kg at an energy density of 6 Wh/kg. It maintained normal power output even in the challenging harsh environment, which enabled 11,000 uninterrupted charge–discharge cycles at 0°C. This work focuses on the regulation of the interfacial microdomain and the restriction of the degree of freedom of H₂O molecules to boost the ESW of aqueous electrolytes, providing a promising strategy for the advancement of energy storage technologies.

The urgent demand for clean energy solutions has intensified the search for advanced storage materials, with rechargeable alkali-ion batteries (AIBs) playing a pivotal role in electrochemical energy storage. Enhancing electrode performance is critical to addressing the increasing need for high-energy and high-power AIBs. Next-generation anode materials face significant challenges, including limited energy storage capacities and complex reaction mechanisms that complicate structural modeling. Sn-based materials have emerged as promising candidates for AIBs due to their inherent advantages. Recent research has increasingly focused on the development of heterojunctions as a strategy to enhance the performance of Sn-based anode materials. Despite significant advances in this field, comprehensive reviews summarizing the latest developments are still sparse. This review provides a detailed overview of recent progress in Sn-based heterojunction-type anode materials. It begins with an explanation of the concept of heterojunctions, including their fabrication, characterization, and classification. Cutting-edge research on Sn-based heterojunction-type anodes for AIBs is highlighted. Finally, the review summarizes the latest advancements in heterojunction technology and discusses future directions for research and development in this area.

Carbon electrocatalyst materials based on lignocellulosic biomass with multi-components, various dimensions, high carbon content, and hierarchical morphology structures have gained great popularity in electrocatalytic applications recently. Due to the catalytic deficiency of neutral carbon atoms, the usage of single lignocellulosic-based carbon materials in electrocatalysis involving energy storage and conversion presents unsatisfactory applicability. However, atomic-level modulation of lignocellulose-based carbon materials can optimize the electronic structures, charge separation, transfer processes, and so forth, which results in substantially enhanced electrocatalytic performance of carbon-based catalysts. This paper reviews the recent advances in the rational design of lignocellulosic-based carbon materials as electrocatalysts from an atomic-level perspective, such as self/external heteroatom doping and metal modification. Then, through systematic discussion of the design principles and reaction mechanisms of the catalysts, the applications of the prepared lignocellulosic-based catalysts in rechargeable batteries and electrocatalysis are reviewed. Finally, the challenges in improving the catalytic performance of lignocellulosic-based carbon materials as electrocatalysts and the prospects in diverse applications are reviewed. This review contributes to the synthesis strategy of lignocellulose-based carbon electrocatalysts via atomic-level modulation, which in turn promotes the lignocellulose valorization for energy storage and conversion.

ZnO with good lithiophilicity has widely been employed to modify the lithiophobic substrates and facilitate uniform lithium (Li) deposition. The overpotential of ZnO-derived Li anode during cycling depends on the lithiophilicity of both LiZn and Li₂O products upon lithiation of ZnO. However, the striking differences in the lithiophilicity between Li₂O and LiZn would result in a high overpotential during cycling. In this research, the Al₂O₃/nZnO (n ≥ 1) hybrid layers were precisely fabricated by atomic layer deposition (ALD) to regulate the lithiophilicity of ZnO phase and Li₂O/LiZn configuration—determining the actual Li loading amount and Li plating/stripping processes. Theoretically, the Li adsorption energy (E_a) values of LiZn and Li₂O in the LiZn/Li₂O configuration are separately predicted as −2.789 and −3.447 eV. In comparison, the E_a values of LiZn, LiAlO_2, and Li₂O in the LiZn/LiAlO₂/Li₂O configuration upon lithiation of Al₂O₃/8ZnO layer are calculated as −2.899, −3.089, and −3.208 eV, respectively. Importantly, a novel introduction of LiAlO₂ into the LiZn/Li₂O configuration could enable the hierarchical Li plating/stripping and reduce the overpotentials during cycling. Consequently, the Al₂O₃/8ZnO-derived hybrid Li-metal anode could exhibit electrochemical performances superior to these of ZnO-derived Li anode in both symmetrical and full cells paired with a LiNi_0.6Co_0.2Mn_0.2O₂ (NCM622) cathode.

Solid electrolytes face challenges in solid-state sodium batteries (SSSBs) because of limited ionic conductivity, increased interfacial resistance, and sodium dendrite issues. In this study, we adopted a unique Sn⁴⁺ doping strategy for Na_3.2Zr₂Si_2.2P_0.8O₁₂ (NZSP) that caused a partial structural transition from the monoclinic (C2/c) phase to the rhombohedral (R-3c) phase in Na_3.2Zr_1.9Sn_0.1Si_2.2P_0.8O₁₂ (NZSnSP1). X-ray diffraction (XRD) patterns and high-resolution transmission electron microscopy analyses were used to confirm this transition, where rhombohedral NZSnSP1 showed an increase in the Na2–O bond length compared with monoclinic NZSnSP1, increasing its triangular bottleneck areas and noticeably enhancing Na⁺ ionic conductivity, a higher Na transference number, and lower electronic conductivity. NZSnSP1 also showed exceptionally high compatibility with Na metal with an increased critical current density, as evidenced by symmetric cell tests. The SSSB, fabricated using Na_0.9Zn_0.22Fe_0.3Mn_0.48O₂ (NZFMO), Na metal, and NZSnSP1 as the cathode, anode, and the solid electrolyte and separator, respectively, maintains 65.86% of retention in the reversible capacity over 300 cycles within a voltage range of 2.0–4.0 V at 25°C at 0.1 C. The in-situ X-ray diffraction and X-ray absorption analyses of the P and Zr K-edges confirmed that NZSnSP1 remained highly stable before and after electrochemical cycling. This crystal structure modification strategy enables the synthesis of ideal solid electrolytes for practical SSSBs.

Single-atom catalysts (SACs) have garnered interest in designing their ligand environments, facilitating the modification of single catalytic sites toward high activity and selectivity. Despite various synthetic approaches, it remains challenging to achieve a catalytically favorable coordination structure simultaneously with the feasible formation of SACs at low temperatures. Here, a new type of coordination structure for Pt SACs is introduced to offer a highly efficient hydrogen evolution reaction (HER) catalyst, where Pt SACs are readily fabricated by atomically confining PtCl₂ on chemically driven NO₂ sites in two-dimensional nitrogen-doped carbon nanosheets at room temperature. The resultant Pt SACs form the NO₂–Pt–Cl₂ coordination structure with an atomic dispersion, as revealed by X-ray spectroscopy and transmission electron microscopy investigations. Moreover, our first-principles density functional theory (DFT) calculations show strong interactions in the coordination by computing the binding energy and charge density difference between PtCl₂ and NO₂. Pt SACs, established on the NO₂-functionalized carbon support, demonstrate the onset potential of 25 mV, Tafel slope of 40 mV dec⁻¹, and high specific activity of 1.35 A mg_Pt⁻¹. Importantly, the Pt SACs also exhibit long-term stability up to 110 h, which is a significant advance in the field of single-atom Pt catalysts. The newly developed coordination structure of Pt SACs features a single Pt active center, providing hydrogen binding ability comparable to that of Pt(111), enhanced long-term durability due to strong metal-support interactions, and the advantage of room-temperature fabrication.

Visible and near-infrared photodetectors are widely used in intelligent driving, health monitoring, and other fields. However, the application of photodetectors in the near-infrared region is significantly impacted by high dark current, which can greatly reduce their performance and sensitivity, thereby limiting their effectiveness in certain applications. In this work, the introduction of a C₆₀ back interface layer successfully mitigated back interface reactions to decrease the thickness of the Mo(S,Se)₂ layer, tailoring the back-contact barrier and preventing reverse charge injection, resulting in a kesterite photodetector with an ultralow dark current density of 5.2 × 10⁻⁹ mA/cm² and ultra-weak-light detection at levels as low as 25 pW/cm². Besides, under a self-powered operation, it demonstrates outstanding performance, achieving a peak responsivity of 0.68 A/W, a wide response range spanning from 300 to 1600 nm, and an impressive detectivity of 5.27 × 10¹⁴ Jones. In addition, it offers exceptionally rapid response times, with rise and decay times of 70 and 650 ns, respectively. This research offers important insights for developing high-performance self-powered near-infrared photodetectors that have high responsivity, rapid response times, and ultralow dark current.