JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Ruifeng Xu,Ke Wang,Jiaxin Liu,Zhongkang Cao,Wenbo Wang,Xu Zhang,Bingjun Yang,Juan Yang,Xianfeng Fan,Tongtong Yu,Pengjun Ma
The replacement of the oxygen evolution reaction (OER) with the urea oxidation reaction (UOR) coupled with the hydrogen evolution reaction (HER) in water electrolysis systems is regarded as a highly promising strategy for reducing hydrogen production energy consumption, enhancing hydrogen efficiency, and even effectively treating urea wastewater. However, the design and fabrication of UOR catalysts in the UOR coupled HER catalytic water electrolysis system remains one of the significant challenges. Herein, we employed a facile, operable, and practical solid-state reaction method to synthesize two representative types of transition metal phosphosulfide (MPS 3 ) catalysts, and the intrinsic and structural characteristics of these catalysts were systematically characterized. Subsequently, the MPS 3 catalyst was deposited onto a nickel foam substrate (NF) to obtain the MPS/NF catalytic electrode. The UOR and OER performance of the MPS 3 /NF catalytic electrode was evaluated to elucidate the competitive mechanisms of UOR and OER within the MPS 3 catalyst. Results indicated that the UOR driving potentials required for NiPS 3 /NF and FePS 3 /NF electrodes were individually reduced by 101 mV and 33 mV compared to the corresponding OER driving potentials under the condition of 100 mA/cm 2 , and NiPS 3 /NF and FePS 3 /NF electrodes could even achieve large UOR current density of 300 mA/cm 2 at potentials as low as 1.630 V (vs. RHE) and 1.647 V (vs. RHE), respectively. In-situ Raman spectroscopy combined with XPS analysis revealed distinct catalytic pathways for NiPS 3 and FePS 3 . During catalysis, NiPS 3 undergoes surface reconstruction to form γ-NiOOH, which exhibited superior selectivity toward urea oxidation, whereas FePS 3 predominantly generated β-FeOOH, whose activity was compromised by competing oxygen evolution, thereby conferring weaker UOR selectivity compared with NiPS 3 . For the UOR-coupled HER whole-cell urea electrolysis assessment, the NiPS 3 /NF and FePS 3 /NF whole-cell attained urea degradation efficiencies of 89.04 % and 69.61 %, respectively. This work provided a novel strategy and practical approach for the development of novel, efficient, and cost-effective MPS 3 catalysts for UOR coupled with HER in the treatment of urea wastewater for synergistic hydrogen production.
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ACS Catalysis
·
2025
·
IF 13.1
Rui Zhai,Zhenyu Wang,Chang Huang,Chao Zeng,Mengyue Gu,Tianqi Wang,Fanqi Bu,Shaobin Wang,Jinying Zhang
Phosphorus has various crystallographic structures and variable phosphorus-derived structures, which have attracted much attention due to its unique properties. One-dimensional phosphorus structures with atomic substitution in the phosphorus lattice are extremely favored due to their high specific surface area and stable single-atom dispersion. The precise crystal structures and single atomic substitution positions are crucial factors to understand the mechanism of single-atom effects but remain a big challenge. Herein, single crystals composed of 1D zigzag linear phosphorus selenium chains (ZLP-Se) have been produced and characterized by SC-XRD to be P18.56Se1.44 with a space group of Pnma (CSD-2348033). The exact Se substitution positions were further ascertained by calculations of the whole thermodynamic stability phase diagram to have three types of substitution patterns (Se1/P1 mixed occupied positions with intervals of 3Se+2P, 1Se+4P, and 1Se+1P+1Se+2P). The selenium-rich crystal plane (-10-1) has been demonstrated to significantly enhance CO2 adsorption and C−C coupling to obtain ethylene (C2H4). A high photocatalytic CO2 reduction performance (18.0 μmol g−1 h−1, 97.0% electron selectivity for C2H4) has been achieved by the ZLP-Se with the Ag cocatalyst. The adsorption of CO2* and CO* was found to be much stronger on the Se-rich surface of ZLP-Se. The CO* intermediates were found to be energetically favored for protonation and subsequent asymmetrical C−C coupling to produce C2H4, with COCHO* intermediates detected by in situ DRIFTS. The electron was also demonstrated by in situ XPS to transfer from Se and Ag to P under Xe lamp irradiation, confirming the electronic localization effect of ZLP-Se to yield C2H4.
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CHINESE CHEMICAL LETTERS
·
2025
·
IF 8.9
Shanshan Wang,Junhao Chen,Kui Qu,Xingyun Li,Hao Wang,Qingchi Xu,Jian Weng,Jun Xu
Unravelling the mechanism of electronic state evolution is ultimately important when attempting to functionalize two dimensional (2D) materials through electronic state regulation. However, there is still a lack of understanding in how the individual local functionalized regions could influence the entire 2D-layered property. Herein, we report the observation of surface electronic behavior during these functionalization process when utilizing the electron-deficient aluminium ion (Al 3+ ) to passivate 2D black phosphorus (BP). Interestingly, the local electron density change in response to a certain functionalization can induce the periodic electron density gradient via inductive integration effect and spread over the entire 2D surface layer. Such 2D coupling effect is evidently supported by the combined investigation of in-situ / ex-situ experimental analysis and theoretical calculation, upon the model Al 3+ -BP modulating process. This work discloses the electron-level relationship between the individual and the whole during the functionalization process and therefore provides a direction for precise manipulation of electronic behavior in functionalized 2D materials.
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iScience
·
2025
·Vol. 28
·期 9
·113294
·
IF 4.1
Kangfan Xie,Guoshuai Fu,Ruiqi Xu,Weimi Ding,Guowei Yang,Peng Yu,Jiling Li,Pu Liu
Scalable water electrolysis requires mass-producible electrocatalysts for efficient hydrogen evolution reaction (HER) at high current densities. We developed a pulsed laser fusion method to synthesize Pd-CuInP 2 S 6 composites on graphene or MXene Ti 3 C 2 nanosheets. These catalysts exhibit enhanced charge transfer and abundant active sites, outperforming commercial Pt/C in both acidic (0.5 M H 2 SO 4 ) and alkaline (1 M KOH) electrolytes. Density functional theory (DFT) analysis reveals synergistic HER enhancement via interstitial H and substituted In atoms. The optimized catalysts achieve remarkable overpotentials of −388 and −384 mV at 1,000 mA cm −2 (acid), with Tafel slopes of 61 and 67 mV dec −1 , while demonstrating −455 and −450 mV overpotentials (alkaline) with 152 and 150 mV dec −1 Tafel slopes, respectively. They maintain exceptional stability over 10,000 CV cycles and extended operation at −500 mA cm −2 , significantly surpassing Pt/C durability. This laser fabrication strategy enables scalable production of efficient, stable low-precious-metal catalysts for industrial HER. Chemical energy; Chemical engineering; Electrochemical engineering
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Materials Today
·
2025
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IF 22
Xuexia Lan,Xingyu Xiong,Zhen Li,Yi Zeng,Jing Peng,Renzong Hu,Min Zhu,Hui-Ming Cheng
Highly reliable fast-charging at low temperatures is critical for the advancement of lithium-ion batteries. Despite the safe lithiation potential and high theoretical capacity of a phosphorus-based anode, its decreased Li + transfer leads to reduced capacity utilization and structural variations. We report a black phosphorus (BP)-based anode with fast-charging ability at low temperatures. The design involves BP-Mo particles incorporated with Sn 2 P 2 O 7 , an active Li + reservoir, facilitating fast and uniform Li + diffusion and inducing stable Li 3 P-based solid-electrolyte interphase. The high-mass loaded BP-Mo/Sn 2 P 2 O 7 anode delivers a capacity of 5.6 mA h cm −2 and 751 mA h g −1 at −10°C and 4C, and 4.9 mA h cm −2 and 691 mA h g −1 at −30 °C and 2C, with 79 % and 75 % capacity retention after 300 cycles, respectively. At −50°C, the initial capacity of 616 mA h g −1 retains 92 % after 175 cycles. Under these two conditions, the full cells of BP-Mo/Sn 2 P 2 O 7 paired with LiCoO 2 cathode show comparable stable fast-charging ability at low temperatures, and the pouch cell has a capacity retention of 88 % at −10 °C and 2C after 150 cycles.
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ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Shaowen Dong,JunQin Shi,Hang Li,Rui Zhang,XiaoYang Ma,YongFeng Yang,ChunJuan Cui,Wei Wang,Jinjin Li
Achieving superlubrication on engineered steel surfaces is critical to reduce friction and wear in mechanical engineering. Herein, a lubricant with rapid superlubrication properties is designed by phytic acid (PA) modified black phosphorus (BP) nanosheets (PA-BP) into a mixture of poly (aspartic acid) (PASP) and ethylene glycol (EG) solution (PASP/EG). It is able to achieve a superlubrication state ( µ ≈ 0.0048) at a high contact pressure of 710 MPa on the engineered steel surface and the time to reach superlubrication (tRs) is only 26 s. The addition of PA-BP could reduce wear rate by 96% on the steel surface (1.51×10 −10 mm 3 N −1 m −1 ) compared to the lubrication of PASP/EG. The surface analysis and molecular dynamics simulations show that PA-BP nanosheets are easily adsorbed on the steel surface to form an adsorbent tribofilm. These PA-BP nanosheets occur oxidation during the friction process, which could adsorb water molecules in PASP/EG to form a water layer with a thickness of 18 Å. This leads to the transformation of the shear interface into water layer with low shear strength, thus achieving the rapid superlubrication at high contact pressure. This work provides a new idea for the design of rapid macroscopic superlubrication on engineered steel surfaces for industrial applications.
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NATURE MATERIALS
·
2025
·Vol. 24
·期 9
·1375-1386
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IF 38.5
Zhang Teng,Chen Youxin,He Zhiyan,Liu Qinran,Chen Le,Wang Kai,Chen Wenzhe,Wang Kunchan,Ye Xiaowo,He Zhuoyang,Zhang Yuyang,Zhang Yanming,Liao Chenghao,He Yuan,Gao Wenpei,Zhang Tianyu,Hu Bei,Jiang Shenghao,Shi Fangyuan,Gao Shengguang,Li Xinyue,Chen Changxin
Black phosphorus nanoribbons (BPNRs) with a tunable bandgap and intriguing electronic and optical properties hold strong potential for logic applications. However, efficiently producing high-quality BPNRs with precise control over their size and structure remains a great challenge. Here we achieved high-quality, narrow and clean BPNRs with nearly atomically smooth edges and well-defined edge orientation at high yield (up to ~95%) through the sonochemical exfoliation of the synthesized bulk BP crystals with a slightly enlarged lattice parameter along the armchair direction. The resulting BPNRs have widths centred at 32 nm and can be as narrow as 1.5 nm, with edges consistently aligned along the zigzag direction in measured BPNRs with widths ≤340 nm. The formation of one-dimensional BPNRs with zigzag edges is attributed to the introduction of pre-stress along the armchair direction of the grown bulk BP and the application of suitable sonication conditions. The BPNR bandgap increases as the BPNR width decreases from 83 nm to 13 nm, with a large bandgap of 0.64 eV for a 13-nm-wide BPNR. A typical graphene-contacted field-effect transistor fabricated with a 13-nm-wide and 10-nm-thick BPNR can achieve an on/off ratio of 1.7 × 10 6 , mobility of 1,506 cm 2 V −1 s −1 and on-state channel conductivity of 1,845 µS. The devices also exhibit excellent photodetection performance. Our method opens up a route to produce BPNRs with high material quality and defined edge chirality for fundamental studies and practical applications in electronic and optoelectronic fields.
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Materials Today Physics
·
2025
·
IF 9.7
Chengyan Liu,Qi Zhou,Haisong Liu,Weiwei Li,Peishan Huang,Mengfei Wang,Wenxiang Chen,Mingqiang Hu,Jun-Liang Chen,Shulin Pan,Dong Hu,Song He,Tomohiro Sato,Haiqiao Wei,Lei Miao
SiGe-based thermoelectric (TE) materials exhibit exceptional thermal stability and environmental compatibility for medium-to-high-temperature applications, but their TE performance is limited by inherently high thermal conductivity. This study demonstrates a novel strategy to overcome this limitation by introducing transition metal carbide. Among five investigated candidates (TiC, ZrC, HfC, NbC, TaC), ZrC incorporation proves most effective, achieving a peak zT of ∼1.3 at 873 K and an average zT ( zT avg ) of 0.72 across 323–873 K in n-type SiGe-based materials, representing an obvious improvement over prior reports. This improvement is mainly attributed to a substantial reduction in lattice thermal conductivity ( κ l ), decreasing from 1.98 W m −1 K −1 –1.75 W m −1 K −1 at 873 K compared to the pristine alloy. Phonon dispersion analysis reveals that the extremely low κ l stems from two factors: specific phononic characteristics of ZrC, including a small optical-optical phonon gap, weak acoustic phonon bunching, and low-frequency (∼2.9 THz) acoustic-optical coupling in comparison with other carbides; and a significant phonon spectrum mismatch at the ZrC/SiGe interface. This work advances TE material optimization through targeted dual-phonon-scattering engineering.
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Biomaterials Advances
·
2025
·
IF 6
Xingjian Yan,Han Dong,Liyin Gao,Mengqi Liu,Chunxi Wang
Prostate cancer (PCa) is commonly considered a “cold tumor” due to its immunosuppressive microenvironment. Cold tumors are typically identified by the absence of T-cell infiltration within the tumor, while other immune populations and myeloid cells can be observed in these tumors. To achieve light-heat combined immunotherapy checkpoint inhibitor treatment for castration-resistant prostate cancer, we aimed to transforming “cold tumors” into “hot tumors”. We designed and synthesized a two-dimensional material, selenium-doped black phosphorus (BP), to enhance the photothermal conversion efficiency, and formed Se@BPNSs by liquid-phase exfoliation. To address the issue of enhanced permeability and retention effect, and to achieve efficient targeting, we coated the Se@BPNSs with RM-1 cell membrane derived from mouse prostate cancer cells. By injecting a certain dose of Se@BPNSs into the tumor and irradiating with a 808 nm laser, the Se@BPNSs converted light energy into heat to kill tumor cells at high temperatures while releasing antigens captured by dendritic cells. In addition, we combined the immunotherapy checkpoint inhibitor anti-PD1 to enhance the immune response and promote immune cell infiltration. The successful preparation of Se@BPNSs was verified through material characterization, cell-level and animal-level experiments, and the antitumor effect was meanwhile verified, which further provided guidance for prostate cancer treatment by photothermal synergistic immunotherapy.
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ELECTROCHIMICA ACTA
·
2025
·
IF 5.6
Yijin Shu,Jun Qi,Huanxi Liao,Zeshen Deng,Yongtai He,Lichun Yang
Metal phosphides are promising high-capacity anode materials for lithium-ion batteries (LIBs), yet their practical application is limited by capacity degradation and sluggish reaction kinetics. Here, we develop a plasma-assisted ball milling strategy to synthesize amorphous Sn 4 P 3 -phosphorus composites encapsulated in few-layer graphene (Sn 4 P 3 -P@FLG). This method simultaneously achieves in-situ decomposition of SnP 3 into Sn 4 P 3 and phosphorus and exfoliates expanded graphite into ultrathin FLG (3∼5 layers). The FLG coating enhances electronic conductivity and accommodates volume variations, while the phosphorus matrix suppresses Sn coarsening, collectively ensuring stable conversion reversibility. The optimized Sn 4 P 3 -P@FLG delivers an impressive initial reversible capacity of 1356.2 mAh g -1 at 0.1 A g -1 , with coulombic efficiency of 89.1 %. It exhibits exceptional long-term cyclability 1 A g -1 , retaining 92 % capacity (1125.8 mAh g -1 ) after 400 cycles. Furthermore, a full cell paired with commercial LiFePO 4 maintains 86.1 % capacity (882.4 mAh g -1 ) after 150 cycles at 1 A g -1 , demonstrating practical viability. The high electrochemical performance demonstrates the potential of Sn 4 P 3 -P@FLG as a promising anode material for LIBs.
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Nanoscale Horizons
·
2025
·Vol. 10
·期 3
·561-567
·
IF 6.6
Yu Xing,Haoshen Ye,Guowei Du,Xu Li,Le-Ping Miao,Junchao Zhang,Xiong Luo,Xiyu Chen,Haoran Ye,Aoli Shen,Zhicheng Wang,Yumeng You,Shuai Dong,Linglong Li
The coexistence of electric and magnetic orders with intrinsic coupling, referred to as magnetoelectric coupling in multiferroics, has been extensively studied in oxide materials but remains relatively unexplored in van der Waals materials. Among these, CuCrP2S6 (CCPS) is notable for its emergent antiferromagnetic (AFM) and antiferroelectric (AFE) characteristics. However, investigations into magnetoelectric coupling in CCPS are limited, and the effects of dopants on its magnetic properties have yet to be fully addressed. In this study, we synthesized CuCr1−xFexP2S6 (CCFPS) samples using the chemical vapor transport (CVT) method to investigate the influence of iron doping on the magnetic and nonlinear optical properties of the CCFPS system. Our results indicate that the AFM state is preserved, while the Néel temperature (TN) varies with the doping concentration. First-principles calculations were employed to assess the exchange interactions among magnetic atoms. Notably, for samples with doping concentrations x < 0.5, we observed both magnetic-dielectric coupling and second harmonic generation (SHG) effects. However, these effects were absent at higher doping levels. Furthermore, our analysis revealed a distinct odd–even dependence of SHG, suggesting the presence of interlayer symmetry-breaking coupling. These findings advance our understanding of two-dimensional (2D) multiferroic materials and lay the groundwork for designing and optimizing magnetoelectric coupling materials with enhanced performance.
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iScience
·
2025
·
IF 4.1
Hongwei Su,Qing Guo,Hongtao Li,Alei Li,Yunlei Zhong,Xu Zhang,Lin Geng,Shuai Liu,Liuqi Dong,Xiaohang Pan,Lin Wang,Lixing Kang
Developing low-cost, high-performance metal-free electrocatalysts is crucial for sustainable oxygen evolution reactions (OERs) in alkaline media. Here, we synthesized ultra-long boron phosphide (BP) microwires along the [111] crystal axis with high yield. By controlling temperature and adding Ni, we identified Ni’s role as a flux and transport agent, optimizing BP microwires at 1050°C. Electrical property and band structure analysis revealed BP as a one-dimensional p-type semiconductor with a wide band gap. We constructed an on-chip electrocatalytic microdevice using individual BP microwires to evaluate OER performance. In 1M NaOH, the BP electrode achieved 50 mA cm −2 at an overpotential of 320 mV, outperforming other boron-based catalysts. Additionally, the nanocatalyst exhibited a low Tafel value (88 mV·dec −1 ) and excellent stability. This study offers valuable insights for developing future electrocatalysts and electrochemical reaction models.
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