CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Yixing Luo,Qingsheng Wu,Yongqing Fu,Ming Wen
Built-in electric field (BIEF) in metallic chalcogenide heterostructures has recently attracted significant attention due to its special interfacial electronic structure and appropriate reaction microenvironment for improving electrocatalytic performance. However, constituent dissolution issues and inferior stability of transition metal selenide heterostructure severely inhibit the formed BIEF to support long-term high-activities for ORR and OER toward zinc-air battery (ZAB). Herein, BIEF was established in CoSe 2 -FeSe 2 hetero-nanostructures encapsulated by N-doped carbon shell on N-doped honeycomb carbon (CoSe 2 -FeSe 2 @NC/NHC) for achieving long-term efficient oxygen electrocatalysis. DFT calculation results confirm that the durable BIEF formed in CoSe 2 -FeSe 2 @NC on NHC not only optimizes interfacial electronic structures and surface adsorption energy, but also offers numerous hyperactive interfacial sites during electrocatalytic reactions. Consequently, the designed CoSe 2 -FeSe 2 @NC/NHC exhibits remarkable performance for both ORR ( E 1/2 = 0.87 V) and OER ( E j = 10 mA cm-2 = 1.54 V), enabling superior peak power density and long-term charging-discharging stability in both liquid-state ZAB (184.3 mW cm −2 and 1350 cycles) and flexible all-solid-state ZAB (61.4 mW cm −2 and 195 cycles). The high durability of BIEF in the core–shell hetero-nanostructured electrocatalyst is crucial for long-term highly-active oxygen electrocatalysis in ZAB.
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Surfaces and Interfaces
·
2025
·
IF 6.3
An Jiang,Yaofeng Shi,Feng Gao
The oxygen evolution reaction (OER) confronts significant challenges due to its intricate electron transfer mechanism, which leads to slow reaction kinetics and high energy barriers. Traditional catalysts possess drawbacks of cost and scarcity, limiting their applicability on a large scale. In this study, we developed a heterojunction catalyst via a hydrothermal method, in situ growing Fe 2 NiSe 4 on the surface of NiFePBA (NiFePBA/Fe 2 NiSe 4 ). The built-in electric field (BIEF) generated at the NiFePBA/Fe 2 NiSe 4 heterojunction showed improved catalytic activity for OER, where the interface electron transfer was markedly enhanced. By modulating the degree of selenization, the inner BIEF intensity can be finely tuned, by which the lowest charge transfer resistance (R ct ) value (2.38 Ω) was obtained for NiFePBA/Fe 2 NiSe 4 -40. The optimized NiFePBA/Fe 2 NiSe 4 -40 structure demonstrated better electrocatalytic activity in 1 M KOH, achieving high current densities of 10 mA cm -2 and 100 mA cm -2 at low overpotentials of 275 mV and 350 mV, respectively. Additionally, the catalyst exhibited excellent stability and a low Tafel slope of 62.60 mV dec -1 . Our work provides new guidance and strategy for the development of high-performance OER catalysts.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
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IF 9.7
Jing Li,Chen Yuan,Huiting Xu,Huibin Liu,Junjie Qi,Zhaohua Jiang,Sai Dong,Rongyu Guo,Zhijie Cui,Wenchao Peng,Jiapeng Liu
Conversion-type aqueous copper-selenium (Cu-Se) batteries have gained considerable attention due to their high theoretical capacity, safety and environmental friendliness. However, the multi-electron intermediate conversion reaction of selenium cathode generally possesses sluggish kinetics, which seriously impedes the further development of Cu-Se batteries. Herein, the porous V 2 C@VSe 2 heterostructure (P-V 2 C@VSe 2 ) with built-in electric field (BIEF) were successfully synthesized by the sacrificial template method and in situ selenization strategy, which were used as the selenium host materials for aqueous Cu-Se batteries to effectively enhance the selenium conversion reaction kinetics. The porous structure of P-V 2 C@VSe 2 not only provides faster access for the transport of polyselenide intermediates during electrochemical reactions, but also exposes more catalytic active sites, which in turn improves the catalytic activity of the material. In addition, the built-in electric field generates at the interface of the P-V 2 C@VSe 2 heterostructure facilitates the acceleration of charge transfer and thus improves the kinetics of the redox reaction of selenium. Benefiting from the synergistic effect of the porous structure and the built-in electric field, the Se/P-V 2 C@VSe 2 cathode possessed a discharge specific capacity of 1182.2 mAh g −1 at a current density of 1 A g −1 , which was much higher than those of Se/P-V 2 C (796.6 mAh g −1 ) and Se (597.0 mAh g −1 ) cathodes. In addition, it also maintained a specific capacity of 1054.6 mAh g −1 after 6000 cycles at 10 A g −1 , demonstrating excellent cycling stability. Meanwhile, a series of characterizations and density functional theory calculations were performed to systematically explore the conversion mechanism of aqueous Cu-Se batteries. This work provides promising insights into the construction of high-performance MXene-based catalytic host materials for aqueous Cu-Se batteries.
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ACS Nano
·
2025
·
IF 16
Jing Qin,Xiujuan Wang,Heyang Li,Fangxiang Wang,Ling Chen,Hongya Miao,Fangfang Xing,Shupei Yuan,Ziqi Ye,Xifei Li,Xiaoming He
Transition metal chalcogenides (TMCs) have garnered significant attention as high-capacity anode materials, yet the unconventional role of the Cu collector meditating atomic-level substitution of metal-site cations by Cu4+ ions during electrochemical cycling remains mechanistically unclear. To address this, herein, Cu-doped MoSe2@C ultrathin nanosheets were synthesized via the solvothermal process and carbonization strategies. A systematic investigation was conducted to elucidate the underlying driving forces for Cu4+ substitution at Mo4+ sites and the crucial regulatory effects of solid electrolyte interphase (SEI) formation. The substitution mechanism was elucidated through the Hard and Soft Acid–Base principle, where Cu4+ (classified as a soft acid) demonstrates significantly stronger coordination affinity with Se2– anions (soft bases) compared to the native Mo4+ cations (hard acids). This electrochemical transition is mediated by ether-based electrolytes coupled with the Cu collector, where the in situ formation of a thin, inorganic-rich SEI layer establishes synergistic ion-transport highways for accelerated Na+/Cu4+ co-diffusion. Temperature-dependent studies reveal Arrhenius-type kinetics: charge transfer is kinetically hindered at ≤ 0 °C but thermally activated at 50–70 °C, confirming that interfacial charge transfer requires thermal energy to overcome activation barriers. This work provides a fundamental guideline for designing stable metal chalcogenide electrodes through interface engineering and electrolyte optimization.
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Journal of Energy Storage
·
2025
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IF 9.8
Jialin Wang,Qianqian Zhang,Shanshan Liu,Ye Liu,Xin Yang,Kai Feng
The design and synthesis of high-performanced anode materials is the key to further improve the performance of lithium-ion batteries (LIBs). In this work, in-situ carbon-coated NbO 2.5-x @C anode materials are prepared to realize synergy of hierarchical engineering, heterogeneous engineering, and defect engineering. The NbO 2.5-x @C anode material delivers a high initial discharge specific capacity of 372 mAh/g and a good cycling stability. In addition, in-situ X-ray diffraction (XRD) and ex-situ X-ray photoelectron spectroscopy (XPS) measurements reveal the mechanism of transformation reaction and (de)intercalation reaction during the charging-discharging processes. This study provides an effective strategy for the design and synthesis of high-performance oxide anode materials for LIBs.
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ACS Photonics
·
2025
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IF 6.7
Haixiao Xu,Yichi Zhang,Yousheng Zou,Zhi Li,Yu Gu
Recent advances in micro- and nanophotonic fabrication techniques have enabled precise control over thermal emissivity, unlocking a variety of intriguing applications. With self-adaptive features, dynamic tunability promises transformative potential but often depends on specialized materials with infrared optical properties responsive to external stimuli, limiting material choices and design flexibility. Herein, we introduce a new framework for dynamic emissivity modulation that exploits the phase-dependent energy dissipation, where the electromagnetic phase controls the amplitude of the total electric field and, consequently, the dissipation rate of the thermal emitter near metallic surfaces. Employing a bilayer system composed of Ag2Se quantum dots (QDs) and a LiF spacer layer on a metallic substrate, we experimentally demonstrate a tunable range of spectral emissivity (Δϵλ) of ∼0.7 and a tunable range of total integrated emissivity in the 8–13 μm waveband (Δϵ) of ∼0.5. The theoretical result also suggests that a dynamic range of the total emissivity as large as 0.6 is feasible by replacing the spacer layer with thermal-responsive polymers, electroelastic materials, magnetoelastic materials, or other phase modulating layers. This design provides a versatile platform for integrating various stimuli-responsive materials to enable dynamically tunable thermal emissivity, paving the way for advanced applications in self-adaptive thermal management and smart thermal systems.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-12
·
IF 15.7
Zong Jingui,Liang Yazhan,Liu Fan,Zhang Mingzhe,Song Kepeng,Feng Jinkui,Xi Baojuan,Xiong Shenglin
Compared with lithium-ion batteries (LIBs), sodium-ion batteries (SIBs) are an alternative technology for future energy storage due to their abundant resources and economic benefits. Constructing various defects is considered to be a common viable means of improving the performance of sodium storage. However, it is of significance to thoroughly scrutinize the formation mechanism of defects and their effects and transition during the charge–discharge process. Here, twin structures are introduced into ZnSe 0.7 Te 0.3 nanocrystals by doping of Te heteroatoms. The Te dopants are visualized to locate in the lattices of ZnSe by spherical aberration electron microscopy. The formation of twin structures is thermodynamically promoted by Te heteroatoms partially replacing Se based on the theoretical calculation results. Moreover, calculation results show that with the increase of twin boundaries (TBs), the sodium diffusion energy barrier is greatly reduced, which helps the kinetics of sodium ion diffusion. In the connection, the composition and amount of TBs are optimized via tuning the doping level. The combined effect of point defects and twin structures greatly improves the sodium storage performance of ZnSe 0.7 Te 0.3 @C. Our work reveals the mechanism of the point defect on the twin plane defect and systematically investigates their effect on the electrochemical performance.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-12
·
IF 15.7
Fu Hui,Wu Yaqiang,Guo Yuhao,Sakurai Takuya,Zhang Qianqian,Liu Yuanyuan,Zheng Zhaoke,Cheng Hefeng,Wang Zeyan,Huang Baibiao,Wang Qian,Domen Kazunari,Wang Peng
Solar-driven photocatalytic water splitting offers a sustainable pathway to produce green hydrogen, yet its practical application encounters several challenges including inefficient photocatalysts, sluggish water oxidation, severe reverse reactions and the necessity of separating produced hydrogen and oxygen gases. Herein, we design and develop a photocatalytic system composed of two separate reaction parts: a hydrogen evolution cell containing halide perovskite photocatalysts (MoSe 2 -loaded CH(NH 2 ) 2 PbBr 3-x I x ) and an oxygen evolution cell containing NiFe-layered double hydroxide modified BiVO 4 photocatalysts. These components are bridged by a I 3 − /I − redox couple to facilitate electron transfer, realizing efficient overall water splitting with a solar-to-hydrogen conversion efficiency of 2.47 ± 0.03%. Additionally, an outdoor scaled-up setup of 692.5 cm 2 achieves an average solar-to-hydrogen conversion efficiency of 1.21% during a week-long test under natural sunlight. By addressing major limitations inherent in conventional photocatalytic systems, such as the cooccurrence of hydrogen and oxygen in a single cell and the resultant severe reverse reactions from hydrogen and oxygen recombination, this work introduces an alternative concept for photocatalytic system design, which enhances both efficiency and practicality.
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GREEN CHEMISTRY
·
2025
·Vol. 27
·期 17
·4540-4550
·
IF 9.2
Yang Zhao,Ruguang Wang,Jisi Li,Jiaxin Guo,Quanlu Wang,Zheng Lv,Pengfei Yin,Tao Ling
Single-atom catalysts towards the oxygen reduction reaction (ORR) often suffer from unsatisfactory activity and poor stability. Herein, for the first time, we successfully modulated the electronic structure of the Mn–N–C catalyst by introducing chalcogen oxygen groups (XO2, X = S, Se, Te), which induce changes in the Mn–N bond length in the MnN4 structure, thereby modulating the electronic structure of the metal center Mn. The experimental results demonstrate that the introduction of XO2 groups results in the rearrangement of Mn 3d electrons, which can be strongly correlated with the ORR activity of the Mn–N–C catalysts, among which the SeO2 modification increases the kinetic current density of the Mn–N–C catalyst achieving a half-wave potential (E1/2) of 0.79 V versus the reversible hydrogen electrode, approaching that of Fe–N–C catalysts along with significant stability in acidic media. The promising performance of the Mn–N–C catalyst as a PGM-free cathode was confirmed through fuel cell testing. First-principles calculations demonstrate that the introduced XO2 group downshifts the d-band center of the Mn center, thus successfully optimizing the adsorption of oxygen intermediates. This finding significantly facilitates the activity enhancement of Mn–N–C catalysts via the construction of a geometric structure–electronic structure–catalytic property relationship.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-12
·
IF 15.7
Fan Xiulian,Yi Jiali,Deng Bin,Zhou Cong,Zhang Zejuan,Yu Jia,Li Weihan,Li Cheng,Wu Guangcheng,Zhou Xilong,Sun Tulai,Zhu Yihan,Zhou Jian,Xia Juan,Wang Zenghui,Lai Keji,Peng Zheng,Li Dong,Pan Anlian,Zhou Yu
The experimental realization of single-crystalline high-κ dielectrics beyond two-dimensional (2D) layered materials is highly desirable for nanoscale field-effect transistors (FETs). However, the scalable synthesis of 2D nonlayered high-κ insulators is currently limited by uncontrolled isotropic three-dimensional growth, hampering the achievement of simultaneous high dielectric constants and low trap densities for small film thicknesses. Herein, we show a 2D edge-seeded heteroepitaxial strategy to synthesize ultrathin nonlayered 2D CaNb 2 O 6 nanosheets by chemical vapor deposition, exhibiting high-crystalline quality, thickness-independent dielectric constant (~ 16) and breakdown field strength up to ~ 12 MV cm −1 . The MoS 2 /CaNb 2 O 6 FETs exhibit an on/off ratio of over ~ 10 7 , a subthreshold swing down to 61 mV/dec and a negligible hysteresis. This work suggests a universal 2D edge-seeded heteroepitaxy and slow kinetic strategy for the scalable growth of 2D nonlayered dielectric and demonstrates 2D CaNb 2 O 6 nanosheets as promising dielectrics for facilitating 2D electronic applications.
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Science Advances
·
2025
·Vol. 11
·期 27
·
IF 12.5
Shenghong Ren,Heyang Chen,Huangliu Fu,Haoran Huang,Tian-Ran Wei,Xun Shi,Xiuyan Li
Ductile polycrystals are usually metals with high-symmetry structures that provide multiple slip systems to coordinate the synergetic deformation of adjacent grains. However, while exceptional plasticity was recently discovered in a series of low-symmetry semiconductors, their deformation mechanism remains mysterious. Here, taking monoclinic Ag 4 SSe as a case study, we show that the inherent high-symmetry anion sublattice with a quasi–body-centered cubic (bcc) structure is embedded in the monoclinic matrix. This, coupled with the highly diffuse cations, results in multiple slip systems and is responsible for the superior plasticity as normally unexpected in low-symmetry structures. We observe typical slip systems conforming with those of the bcc structure by experiment. This finding clarifies the deformation mechanism of Ag 2 S-based low-symmetry semiconductors and sheds light on future exploration of ductile inorganic semiconductors.
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OPTICS EXPRESS
·
2025
·Vol. 33
·期 11
·22588-22597
·
IF 3.3
Tingting Zhang,Qing Ma,Qingping Li,Lanting Huang,Yuqiong Feng,Hongwei Duan,Xinlei Chen,Qinghua Li,Xiao Jin,Jinke Bai,Jinke Bai,Bing Xu,Bing Xu
Heavy metal-free ZnSe-based core-shell quantum dots (QDs) are promising emitting material for achieving violet-blue luminescence. Investigating the temperature-dependent variations in the photoluminescence (PL) properties of ZnSe-based QDs will enhance our understanding of the intrinsic factors that influence their diverse luminescence characteristics. Here we select the optimally synthesized ZnSe core QDs with three diameters (4.1, 5.2, and 8.3 nm) and ZnSe/ZnS core-shell QDs to study their temperature-dependent photoluminescence properties. As the sample temperature is increased, the PL intensity decreases, the emission energy redshifts, and the spectral become broader. We observe a reduction in the exciton- longitudinal optical (LO)-phonon coupling constant from 21.7 meV to 16.1 meV as the diameter of ZnSe core QDs increased from 4.1 nm to 8.3 nm. This decrease is associated with a narrower homogeneous broadening of the emission spectrum. Besides, the epitaxial growth of a ZnS wide bandgap shells onto the ZnSe core QDs can effectively isolate the photogenerated excitons away from the inorganic-organic interface, thus reducing the PL peak width and increasing the exciton binding energy of the QDs. Our research provides a valuable addition to the existing studies on the photoluminescence properties of ZnSe-based core-shell QDs.
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