APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Shihu Cao,Shugang Zheng,Tianci Liu,Jinhao Liu,Yaqi Yin,Dan Feng,Yunqing Liu,Dayi Qian,Jiangwei Shang,Xiuwen Cheng
Herein, we identified interfacial oxygen vacancy-metal (O V -Ni) dual-sites within a NiFe 2 O 4 /Ni@NC composite as the definitive structural origin for dictating the selective evolution of singlet oxygen ( 1 O 2 ) from peroxymonosulfate (PMS) activation. The catalyst was fabricated via in-situ pyrolysis of a Ni-MOF on NiFe 2 O 4 nanoparticles, and its mechanism was elucidated through a combination of in-situ spectroscopy, kinetic analysis, and density functional theory (DFT) calculations. This 1 O 2 -driven catalysis achieved an 11-fold enhancement in the levofloxacin degradation rate, with the interfacial synergy lowering the non-radical pathway’s energy barrier by 0.037 eV. We conclude that these engineered dual-sites deterministically control reaction selectivity, as proven by the first experimental trapping of a surface-bound 1 O 2 precursor. This work establishes a design blueprint for advanced non-radical catalysts by transforming the approach from serendipitous discovery to predictable, interface-driven design.
研究领域:
环境催化
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材料化学
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物理化学
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纳米催化
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水处理技术
✓ 已验证
产品关联
DOI
高影响因子
ChemSusChem
·
2020
·Vol. 13
·期 18
·5004-5014
·
IF 7.962
Xinyang Ji,Yongxia Zhang,Zhuo Ma,Yunfeng Qiu
Graphical Enhanced, three ways ! Oxygen vacancy-rich Ni/NiO nanosheets with Schottky heterointerface are protected by ultrathin N-doped carbon layer and display high urea oxidation reaction (UOR) performance. Charge polarization of active sites at Schottky interface, enhanced conductivity owing to the presence of defective energy level, and synergistic effect between anti-corrosion carbon layer and active sites are responsible for the enhanced specific UOR activity and long-term stability. H 2 production via electrocatalytic water splitting is greatly hindered by the sluggish oxygen evolution reaction (OER). The urea oxidation reaction (UOR) draws specific attention not only because of its lower theoretical voltage of 0.37 V compared with OER (1.23 V), but also for treating sewage water. Herein, Ni/NiO nanosheets with an ultrathin N-doped C layer containing a Schottky Ni and NiO heterointerface is constructed. Because of the self-driven charge redistribution at the heterointerface, janus charge domains are successfully created to drive the cleavage of urea molecules. Meanwhile, the synergistic effect between N-doped C and Ni/NiO restrains the deactivation of active sites in alkaline solution. The catalyst displays 1.35 V for UOR at 10 mA/cm 2 , 0.27 V lower than that of OER. The final potential increase is only 2 mV after long-term stability test of 12 h for UOR, much smaller than the uncoated sample (38 mV). The present work shows that C-coated transition metal nanomaterials with oxygen vacancies and a Schottky heterointerface are promising candidates for simultaneously boosting UOR with both high activity and long-term stability.
研究领域:
材料科学
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电化学
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催化
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纳米技术
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能源材料
✓ 已验证
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2025
·
IF 8.3
Jingwen Ma,Ruiting Wang,Tianai Zhang,Ying Tian,Jinhao Liu,Junbin Li
Urea-assisted hydrogen production is an emerging hydrogen production technology that offers a new approach to the efficient and clean production of hydrogen energy. The low energy consumption urea oxidation reaction replaces the high energy consumption oxygen evolution reaction (OER), significantly reducing the energy consumption of hydrogen production and achieving the resource utilization of pollutants in wastewater (including urea). It is expected to become an important pathway for green hydrogen production with both economic and environmental benefits. The novel composite catalyst Ru/NiMoOx@NC, prepared by supporting ruthenium on a nitrogen-doped carbon-coated nickel-molybdenum oxide support, exhibits highly efficient bifunctional catalytic activity, enabling it to efficiently catalyze the hydrogen evolution reaction (HER) and promote the urea oxidation reaction (UOR). Specifically, the introduction of trace ruthenium synergizes with the nickel-molybdenum bimetallic oxide to accelerate H 2 generation. The nitrogen-doped carbon substrate enhances the catalyst's electrical conductivity. Additionally, the incorporation of Mo reduces CO poisoning of Ni active sites during the UOR, further to enhance the catalyst's stability. By varying the loading of Ru, materials with optimal and superior properties are obtained. The Ru/NiMoO x @NC catalysts demonstrate excellent UOR (1.37 V vs. RHE@25 mA cm −2 ; 1.39 V vs. RHE@100 mA cm −2 ) and HER (−98 mV@25 mA cm −2 ) performance under alkaline conditions. The current density of the Ru/NiMoOx@NC electrode remains almost unchanged after cyclic voltammetry (CV) tests and chronoamperometric durability tests, exhibiting excellent catalytic stability. In this system, Ru/NiMoOx@NC serves as both the anode and cathode of the urea-assisted hydrogen production battery, which only requires a voltage of 1.56 V to achieve an output current density of 50 mA cm −2 and demonstrates excellent overall water electrolysis stability. This work provides new insights for the design of bifunctional catalysts for urea-assisted hydrogen production.
研究领域:
能源技术
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催化
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材料科学
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电化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Jiabing Luo,Yan Zhou,Xingzhao Wang,Yufeng Gu,Wanli Liu,Shutao Wang,Jun Zhang
We report the synthesis and electrocatalytic properties of a CoMoO 4 -CoP heterostructure anchored on a hollow polyhedral N -doped carbon skeleton (CoMoO 4 -CoP/NC) for water-splitting applications. The preparation involved the anion exchange of MoO 4 2- to the organic ligand of ZIF-67, the self-hydrolysis of MoO 4 2- , and NaH 2 PO 2 phosphating annealing. CoMoO 4 was found to enhance thermal stability and prevent active site agglomeration during annealing, while the hollow structure of CoMoO 4 -CoP/NC provided a large specific surface area and high porosity that facilitated mass transport and charge transfer. The interfacial electron transfer from Co to Mo and P sites promoted the generation of electron-deficient Co sites and electron-enriched P sites, which accelerated water dissociation. CoMoO 4 -CoP/NC exhibited excellent electrocatalytic activity for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in 1.0 M KOH solution, with overpotentials of 122 mV and 280 mV at 10 mA cm −2 , respectively. The CoMoO 4 -CoP/NC‖CoMoO 4 -CoP/NC two-electrode system only required an overall water splitting (OWS) cell voltage of 1.62 V to achieve 10 mA cm −2 in an alkaline electrolytic cell. In addition, the material showed comparable activity to 20% Pt/C‖RuO 2 in a pure water home-made membrane electrode device, demonstrating potential for practical applications in proton exchange membrane (PEM) electrolyzers. Our results suggest that CoMoO 4 -CoP/NC is a promising electrocatalyst for efficient and cost-effective water splitting.
研究领域:
材料科学
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电化学
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催化
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能源材料
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF POWER SOURCES
·
2023
·
IF 9.2
Xiaoyu Yang,Ying Qi,Peng Wei,Qixu Hu,Jian Cheng,Yahong Xie
Carbon-based CsPbI 2 Br perovskite solar cells (C–PSCs) have the advantages of low cost and stable performance, but the poor contact and energy mismatch between the perovskite layer and the carbon electrode lead to low power conversion efficiency (PCE). In this work, uniform spindle-shaped Fe 3 O 4 @NC composites have prepared by calcining Fe-based metal organic framework (Fe-MOF) NH 2 -MIL-88B(Fe), which has synthesized by solvothermal reaction using 2-aminoterephthalic acid as nitrogen and carbon sources. Using Fe 3 O 4 @NC composite and UV-Ozone treated Fe 3 O 4 @NC composite (Fe 3 O 4 @NC UVO) as the interfacial layer between the perovskite layer and the carbon electrode, the devices with a structure of FTO/SnO 2 /CsPbI 2 Br/interfacial layer/Carbon exhibit a maximum PCE of 12.25%, which is about 19.28% higher than that of the pristine device. The improved optoelectronic performance is mainly attributed to more matched energy level, denser interface contact, better carrier separation performance and better conductivity. After 19 days of storage at room temperature and ambient humidity, Fe 3 O 4 @NC UVO device has retained 87% of the initial PCE. This work provides a simple and effective strategy to improve the PCE and stability of carbon-based CsPbI 2 Br PSCs with Fe-MOFs-derived carbon materials .
研究领域:
材料科学
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可再生能源
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光伏技术
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Kungang Chai,Shizhao Zhang,Hongjie Liu,Shaopeng Wang,Zhenghua Chen,Kefu Yu,Liwei Wang
Higher resistance is exceptionally detrimental to metal oxide-based electrochemical sensors' detection performances that depend on their electrical conductivity. Herein, guided by the synergistic effect of the heterophase boundary, a hollow core–shell combination with a double-layered structure was engineered via hydrolysis strategy, namely nitrogen-doped carbon hollow nano-microspheres (N C HNMs) coated with SnO 2 outer layer (N C@SnO 2 HNMs), then applied for high-performance electrochemical sensing. Advantages including large surface area and strong electronic coupling of Sn-C bond on the boundary facilitated the adsorption of target molecules and electron transferring across the composites, achieving efficient quantitative identification. Density functional theory (DFT) calculation demonstrated the motivation of the charge accumulation at the interface due to the formation of the Sn-C bond, which acted as a bridge for charge transfer. Unsurprisingly, the N C@SnO 2 HNMs-based electrode showed an excellent performance toward dopamine (DA), such as favorable DA selectivity, a lower limit of detection, and a wide linear detection range. Moreover, the electrode material could be applied to the microsensor for in-situ DA detection in artificial sweat.
研究领域:
材料科学
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电化学
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纳米技术
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传感器
✓ 已验证
产品关联
DOI
高影响因子
CARBON
·
2022
·
IF 11.307
Bin Li,Biao Ma,Mengying Wei,Yang Li,Xiaobin Fan,Fengbao Zhang,Guoliang Zhang,Qing Xia,Wenchao Peng
Recycle of the spent lithium-ion batteries (LIBs) can reuse the toxic heavy metals for the synthesis of useful materials. In this study, the cobalt metal is obtained by recycling the cathodes of spent LIBs, which is then used as cobalt source for the synthesis of highly porous Co-NC composites. Attributing to the addition of EDTA-2Na and NaNO 3 as chelate agent and activation agent respectively, very large surface areas (>3700 m 2 /g) and highly porous structure can be achieved. These composites can activate peroxymonosulfate (PMS) effectively for the degradation of bisphenol A (BPA) in aqueous solution. The optimized Co-NC/PMS system also shows good performance in a wide pH range and great tolerance to different inorganic ions and NOMs. Radical scavenging experiments and EPR results prove that 1 O 2 is the only functional reactive oxidation species (ROS) for BPA degradation. A generation route of PMS – *OH – *O – 1 O 2 for 1 O 2 is also simulated and proved by DFT calculation. This work provides a novel way to synthesize effective catalysts for PMS activation from the environmental wastes.
研究领域:
环境科学
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材料科学
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催化
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废物管理
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Chao Feng,Yuehong Xie,Shanshan Qiao,Yuan Guo,Shiang Li,Li Zhang,Wei Wang,Jide Wang
We used a simple MOFs-assisted synthesis strategy based on the encapsulation and in-situ carburizing reaction of Cu-based metallic organic frameworks (NENU-5) to synthesize porous nano-octahedral materials, MoWN/MoWC@N C Ts (T = 700, 800, and 900). Together with the vapor deposition strategy, the volatile nitrogen species from the pyrolysis of dicyandiamide were captured by the nano-octahedral materials, and formed tungsten-molybdenum-based carbonitride nanocrystals encapsulated in nitrogen-doped carbon. The porous nano-octahedron has a unique heterostructure composed of Mo 2 N/MoC/W 2 N/WC. The representative MoWN/MoWC@N C 800 showed trifunctional electrocatalytic activity in oxygen reduction reaction/oxygen evolution reaction/hydrogen evolution reaction (ORR/OER/HER) in an alkaline medium (0.1 M KOH). The total oxygen electrode activity index ΔE = 0.795 V (vs. RHE) was found in OER/ORR, and the material also exhibits excellent HER performance. The minimum potential of −0.17 V (vs. RHE) was provided at a current density of −10 mA cm −2 . MoWN/MoWC@N C 800 showed excellent cycle stability and durability in ORR/OER/HER with the same electrolyte (0.1 M KOH). More importantly, MoWN/MoWC@N C 800 could be used to construct high-performance zinc-air batteries and sued for driving electrocatalytic water splitting in a self-powered manner. The successful preparation of the materials indicate that the synthetic strategy provides new reference ideas for developing functional materials with high catalytic properties for various applications.
研究领域:
材料科学
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电化学
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催化科学
✓ 已验证
DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-10
·
IF 14.7
Yin Shuhu,Chen Long,Yang Jian,Cheng Xiaoyang,Zeng Hongbin,Hong Yuhao,Huang Huan,Kuai Xiaoxiao,Lin Yangu,Huang Rui,Jiang Yanxia,Sun Shigang
Replacement of expensive and rare platinum with metal–nitrogen–carbon catalysts for oxygen reduction reactions in proton exchange membrane fuel cells is hindered by their inferior activity. Herein, we report a highly active iron-nitrogen-carbon catalyst by optimizing the carbon structure and coordination environments of Fe-N 4 sites. A critical high-temperature treatment with ammonium chloride and ammonium bromide not only enhances the intrinsic activity and density of Fe-N 4 sites, but also introduces numerous defects, trace Br ions and creates mesopores in the carbon framework. Notably, surface Br ions significantly improve the interaction between the ionomer and catalyst particles, promoting ionomer infiltration and optimizing the O 2 transport and charge transfer at triple-phase boundary. This catalyst delivers a high peak power density of 1.86 W cm −2 and 54 mA cm −2 at 0.9 V iR-free in a H 2 -O 2 fuel cells at 80 °C. Our findings highlight the critical role of interface microenvironment regulation.
研究领域:
电化学
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催化
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能源材料
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燃料电池
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Yuan Ma,Nanpu Cheng,Chunhong Li,Muhammad Aizaz Ud Din,Lan Zhao,Nengcong Pan,Yuhan Lei
The development of low-platinum electrocatalysts with high activity in alkaline media is critical for sustainable and cost-effective hydrogen production. In this study, we report a dual-phase engineering strategy to synthesize Pt-CoSe 2 nanoparticles embedded in nitrogen-doped carbon (Pt-CoSe 2 @NC) via controlled pyrolysis of ZIF-67. The resulting catalyst features hierarchical porosity and a 3D conductive network that confines ultrafine Pt particles and enhances interfacial charge and mass transfer. Strong Pt-CoSe 2 interactions induce electron redistribution, elevating cobalt oxidation states and optimizing hydrogen adsorption energetics. Nitrogen doping and surface-oxygenated Co species further boost performance. The optimized Pt-CoSe 2 @NC catalyst exhibits an overpotential of 37.4 mV at 10 mA cm −2 , a Tafel slope of 60.4 mV dec -1 , and remains over 90 % of its initial current density after 24 h in 1 M KOH. Density functional theory (DFT) calculations reveal a shift in the d -band center of Pt due to Pt-CoSe 2 interface formation, leading to near-thermoneutral hydrogen adsorption energy. This work integrates MOF-derived structural control with electronic interface modulation, offering a generalizable blueprint for designing efficient, low-noble-metal HER catalysts.
研究领域:
材料科学
·
电催化
·
能量存储与转换
·
纳米材料
·
密度泛函理论
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Shengzhi He,Jingyu Wang,Chunwen Sun
Oxygen reduction reaction (ORR) serves as the foundation for various electrochemical energy storage devices. Fe/N C catalysts are expected to replace commercial Pt/C as oxygen electrode catalysts based on the structural tunability at the atomic level, abundant iron ore reserves and excellent activity. Nevertheless, the lack of durability and low active site density impede its advancement. In this work, a durable catalyst, Cu Fe/N C, for ORR was prepared by modulating the interfacial composition and electronic structure. The introduction of Cu nanoclusters partially eliminates the Fenton effect from Fe and optimizes the electron structure of Fe N x , thereby effectively enhancing the long-term durability and activity. The prepared Cu Fe/N C exhibits a half-wave potential ( E 1/2 ) of 0.90 V and superior stability with a decrease in E 1/2 of only 20 mV after 10,000 cycles. The assembled alkaline Zinc-Air batteries (ZABs) with Cu Fe/N C exhibit an open-circuit potential of 1.458 V. At a current density of 5 mA cm −2 , the batteries are capable of operation for 600 h with a stable polarization. This Cu Fe/N C may promote the practical application of novel and renewable electrochemical energy storage devices.
研究领域:
电化学
·
催化
·
能量存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Xiaoli Peng,Long Yuan,Shilan Li,Shengdong Jing,Yaozhu Tian,Zhu Luo,Yufei Zhang,Haosen Fan
Lithium‑sulfur batteries (LSBs) have attracted much attention due to their high theoretical energy density (2600 Wh kg −1 ) and low cost of sulfur cathodes. However, their practical application is hindered by the significant polysulfide shuttle effect and sluggish redox kinetics. To address these challenges, a Co-NC/Nb 2 O 5 heterostructure was successfully prepared through high-temperature annealing of a ZIF-67 precursor followed by hydrothermal growth of Nb 2 O 5 nanocrystals on the surface of Co -embedded and N-doped carbon polyhedrons (Co-NC). The unique structure features a hierarchical conductive framework with uniformly dispersed Nb 2 O 5 nanoparticles and defect-rich carbon matrix, which synergistically enhances sulfur utilization and ion diffusion. Numerous dangling bonds and defective sites exist on the Nb 2 O 5 surfaces, and its Lewis acidic site (Nb 5+ ) can inhibit the solvation and shuttling of LiPSs through strong chemical interactions with the S atoms of polysulfides via Nb-O-S bonds. The catalytic and adsorption mechanisms were explained by density functional theory (DFT) calculations and experimental results. Consequently, LSBs cells equipped with Co-NC/Nb 2 O 5 modified separators demonstrated exceptional electrochemical performance with a rate capability that provides a reversible capacity of 761.8 mAh g −1 at 3 °C. The composite of MOF-derived hollow carbon polyhedra decorated with Nb 2 O 5 nanoparticles ensured fast electron transfer, achieving a reversible capacity of 731.4 mAh g −1 after 500 cycles at 1C and 501.6 mAh g −1 after 1000 long cycles at 2C, with a capacity decay rate of only 0.03 % per cycle. Excellent electrochemical performance was maintained with a high sulfur loading cycling performance of 5 mg cm −2 at a low electrolyte/sulfur condition of 7 μL mg −1 . This work provides new insights into the development of high energy density LSBs and the advancement of next generation energy storage systems through precise electronic structure design at the heterojunction interface.
研究领域:
储能材料
·
电化学
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纳米材料
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表面化学
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催化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）