APPLIED CATALYSIS B-ENVIRONMENTAL
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2026
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IF 19.7
Wenlu Zhang,Yaning Fu,Zhen Feng,Mengyao Huang,Youcai Lu,Qingchao Liu
Mn doping creates symmetry-broken Co δ+ -O-Ru δ− heterointerfaces. • Polarized Ru and Co sites enable catalytic shunting of ORR and OER. • Reversible metal-oxygen bond adaptation accelerates Li 2 O 2 conversion. • The catalyst delivers an ultralow discharge-charge overpotential of 0.37 V. • Li-O 2 cells reach 34,738 mAh g −1 and cycle stably for 208 cycles. Aprotic Li-O 2 batteries require efficient bifunctional oxygen electrocatalysis, yet ORR and OER impose conflicting demands on oxygen-intermediate adsorption and product desorption. Herein, we construct a symmetry-broken Mn-doped Co 3 O 4 /RuO 2 heterointerface on carbon cloth to couple catalytic shunting with self-adaptive interfacial bonding. Mn incorporation reinforces Co-O-Ru coupling and generates asymmetric Co δ⁺ -O-Ru δ⁻ units, as verified by XPS, XAS, and theoretical calculations. The resulting interfacial polarization spatially divides the oxygen-redox pathway: electron-enriched Ru sites preferentially promote O₂ adsorption/activation for ORR, whereas electron-deficient Co sites facilitate Li₂O₂ decomposition/desorption for OER. Meanwhile, in situ Raman spectroscopy and theoretical bond-length analysis reveal reversible metal-oxygen bond elongation/contraction during discharge/charge, enabling temporal adaptation of interfacial bonding to evolving intermediates. This spatial shunting and temporal self-adaptation synergistically mitigate the adsorption-desorption conflict, improve Li 2 O 2 reversibility, and maintain efficient charge-transfer pathways. Consequently, the Mn-Co 3 O 4 /RuO 2 cathode achieves a low overpotential of 0.37 V, a high discharge capacity of 34,781 mAh g −1 , and stable cycling for 208 cycles. This study provides a shunt-adaptive heterointerface strategy for multistep oxygen electrocatalysis. Download: Download high-res image (275KB) Download: Download full-size image
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2026
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IF 19.7
PengJiang Chao,Sheng Zhang,EnZhou Liu,Bing Wang,XiaoXun Ma,Zhuo Li
Bi/Sb dual-doping forms synergistic site pairs in ZnIn 2 S 4 , switching O 2 to Yeager-type adsorption. • Yeager-type enables direct 2e - ORR, suppresses •O 2 - , and boosts H 2 O 2 selectivity. • Bi/Sb-ZIS achieves 2612.6 μmol·g⁻¹·h⁻¹ H 2 O 2 and 91.8% TC degradation for integrated purification. Photocatalytic oxygen reduction provides a sustainable route for green hydrogen peroxide (H 2 O 2 ) synthesis, yet its efficiency is often hindered by slow multi‑step electron transfer and competing side reactions. Here, we engineer the surface microenvironment of ZnIn 2 S 4 through Bi/Sb dual doping, creating spatially and electronically complementary “Bi–Sb synergistic site pairs”. These dual sites collectively steer O 2 into a Yeager adsorption configuration and promote direct one‑step 2e - reduction, shifting the dominacnt ORR mechanism from the conventional, radical-prone two-step route to a highly efficient and selective direct pathway. The optimized catalyst achieves a high H 2 O 2 production rate of 2612.6 μmol·g −1 ·h −1 in simulated antibiotic wastewater while simultaneously degrading 91.8% of tetracycline. Mechanistic studies reveal that this pathway switching originates from the synergistic electron transfer at the dual sites, which not only stabilizes the Yeager‑type adsorption conformation but also largely suppresses the formation of •O 2 - intermediates. This work provides an effective bifunctional photocatalyst for integrated “Pollutant Solutions purification–chemical synthesis” systems and establishes a general design principle for controlling multi‑electron reaction pathways through the rational construction of synergistic active sites. Download: Download high-res image (191KB) Download: Download full-size image Bi/Sb-ZIS promotes Yeager-type O 2 adsorption and direct 2e - ORR, delivering exceptional H 2 O 2 yield and pollutant degradation in a dual-functional photocatalytic system.
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Journal of Water Process Engineering
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2025
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IF 6.7
Lei Zou,Lu Wei,Yubei Liu,Mingjie Huang,Xiangling Zhang,Wenjiao Sang,Shuting Li,Chen Wang,Wei Xiang
The pervasive threat of toxic and stable heavy metal-organic complexes to aquatic ecosystems necessitates efficient decomplexation strategies. In this study, we developed a magnetic field (MF)-enhanced nano zero-valent iron (nZVI) system that activated O 2 for the removal of Cu(II) and chemical oxygen demand (COD) from Cu-complexed wastewater (EDTA-Cu, citrate-Cu, tartrate-Cu). The introduction of MF significantly enhanced Cu-complex destruction and Cu 2+ immobilization, while reducing toxicity and improving biodegradability. Mechanistic studies revealed that nZVI would displace Cu from complexes, reducing free Cu 2+ to Cu 0 on its surface. The resultant Cu 0 , in synergy with Fe 2+ , activated O 2 to generate reactive oxygen species (ROS), which cleaved metal-organic bonds and oxidized organic ligands. MF amplified this process by enhancing paramagnetic O 2 accumulation at nZVI/Cu 0 sites, accelerating ROS production via the O 2 ⟶O 2 •− ⟶H 2 O 2 ⟶•OH pathway, thereby boosting Cu-organic decomplexation and COD removal. Catalyst characterization further revealed that MF promoted Cu 0 dispersion on nZVI, preventing cluster formation and optimizing electron utilization for O 2 activation. As demonstrated by our energy-cost efficiency analysis, the MF/nZVI/O 2 process achieved 1.375–1.785 g Cu /kWh for Cu-organic wastewater treatment, significantly outperforming many previously reported processes. This study introduces a novel MF-assisted nZVI system for efficient treatment of Cu-complexes, offering a promising cost-effective and sustainable solution for practical application.
研究领域:
环境科学
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化学工程
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材料科学
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高影响因子
Scientific Reports
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2025
·Vol. 15
·期 1
·1-14
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IF 3.9
Liu Liming,Lian Hongxia,Deng Heming,Zhang Weixin
Challenges associated with the cathode material of Lithium–oxygen (Li–O 2 ) battery, particularly the sluggish kinetics of oxygen reduction reaction (ORR) and oxygen evolution reaction, as well as the accumulation of discharge product Li 2 O 2 , have hindered its further advancement. Here, an in-situ synthesis strategy was adopted to load a bimetallic Ni–Co metal–organic framework (Ni/Co-MOF) onto MXene (Ti 3 C 2 ) layers. Subsequently, a free-standing and flexible Ni/Co-MOF@Ti 3 C 2 hybrid membrane is prepared via a layer-by-layer self-assembly method, specifically designed for efficient ORR and as a cathode for Li–O 2 batteries. The Ni/Co-MOF@Ti 3 C 2 hybrid membrane integrates the high conductivity, unique two-dimensional layered structure, and excellent mechanical properties of Ti 3 C 2 with the bimetallic active sites of Ni/Co-MOF, exhibiting remarkable ORR catalytic activity in an O 2 -saturated 1 M LiTFSI electrolyte. The structural characteristics of the hybrid membrane provide smoother expansion pathways for Li + and O 2 , effectively promoting the deposition and decomposition of Li 2 O 2 . This not only enhances the electrochemical performance of the Li–O 2 battery but also overcomes the inherent limitations of traditional slurry-based cathode preparation methods. Experimental results demonstrate that Li–O 2 batteries utilizing the Ni/Co-MOF@Ti 3 C 2 hybrid membrane as the cathode achieve an ultra-high capacity of 36,125 mAh/g at a current density of 1000 mA/g, while exhibiting excellent cycle stability (271 cycles with a limited capacity of 1000 mAh/g at 1000 mA/g) and outstanding rate performance. The hybrid membrane’s capacity and cycle performance can be further optimized by controlling its thickness. These promising results offer novel insights into the innovative design of air cathodes for metal–air batteries, and the proposed method provides a new route for the manufacture of high-performance battery cathodes.
研究领域:
材料科学
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电化学
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能源存储与转换
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PubMed
高影响因子
Catalysts
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2025
·Vol. 15
·期 7
·694
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IF 4
Ziyan Mi,Huayun Long,Yuhua Jia,Yue Ma,Cuilan Miao,Yan Xie,Xiaomei Zhu,Jiahui Huang
The development of non-noble metal catalysts for gas-phase propylene epoxidation with H2/O2remains challenging due to their inadequate activity and stability. Herein, we report a Cs+-modified Ni/TS-1 catalyst (9%Ni-Cs/TS-1), which exhibits unprecedented catalytic performance, giving a state-of-the-art PO formation rate of 382.9 gPO·kgcat−1·h−1with 87.8% selectivity at 200 °C. The catalyst stability was sustainable for 150 h, far surpassing reported Ni-based catalysts. Ni/TS-1 exhibited low catalytic activity. However, the Cs modification significantly enhanced the performance of Ni/TS-1. Furthermore, the intrinsic reason for the enhanced performance was elucidated by multiple techniques such as XPS, N2physisorption, TEM,29Si NMR, NH3-TPD-MS, UV–vis, and so on. The findings indicated that the incorporation of Cs+markedly boosted the reduction of Ni, enhanced Ni0formation, strengthened Ni-Ti interactions, reduced acid sites to inhibit PO isomerization, improved the dispersion of Ni nanoparticles, reduced particle size, and improved the hydrophobicity of Ni/TS-1 to facilitate propylene adsorption/PO desorption. The 9%Ni-Cs/TS-1 catalyst demonstrated exceptional performance characterized by a low cost, high activity, and long-term stability, offering a viable alternative to Au-based systems.
研究领域:
催化化学
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化学工程
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材料科学
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多相催化
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绿色化学
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高影响因子
Journal of Materials Chemistry A
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2025
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IF 9.5
Guangqi Zhang,Congcong Dang,Yiping Liu,Rouyan Guo,Lingti Kong,Liancheng Zhao,liming Gao
Li-O2 batteries have emerged as promising contenders for advanced energy storage systems, leveraging their exceptionally high theoretical energy density. Nevertheless, their practical deployment is substantially hindered by rapid capacity degradation and restricted operational durability, primarily attributed to sluggish oxygen reaction kinetics. Here, to modulate kinetic barriers, we propose an approach synergizing structural and electronic advantages by integrating heterointerface engineering and hierarchical nano structuring. A hollow nanobox MoSe2@CuS core-shell heterostructure is developed as a bifunctional oxygen electrode. Such heterostructure could induce a built-in electric field to modulate charge transfer dynamics and the hollow architecture could optimize triple-phase interfacial reactions. Leveraging the synergistic attributes of its components, the MoSe2@CuS-based Li-O2 battery achieves an excellent specific capacity of 16,000 mAh g-1 at 100 mA g-1. Moreover, it demonstrates remarkable cycling durability, sustaining high performance for over 190 cycles at 200 mA g-1 with a restricted capacity of 600 mAh g-1. Density functional theory (DFT) calculations further illustrate the lowered energy kinetic barrier for Li2O2 formation/decomposition induced by MoSe2@CuS core-shell heterostructure. This work pioneers a universal heterointerface engineering strategy through rational design of hierarchical hollow architectures, providing new insights for developing high-performance Li-O2 battery cathodes.
研究领域:
储能
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纳米材料
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电化学
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电池技术
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材料科学
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理论化学
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高影响因子
Nature Communications
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2025
·Vol. 16
·期 1
·1-14
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IF 15.7
Wang Peng,Zhao Danyang,Zhang Peng,Hui Xiaobin,Zhang Zhiwei,Wang Rutao,Wang Chengxiang,Ge Xiaoli,Liu Xiaojing,Li Yuguang C.,Yin Longwei
The metallic phase MoS 2 (1T-MoS 2 ) supported metal-nanocatalyst is an appealing material system for accelerating the redox kinetics of non-aqueous Li | |O 2 batteries. However, the drawbacks associated with the surface orbital steric effect and the internal electron coupling results in a detrimental effect for the stability of 1T-MoS 2 , especially for the interface charge transfer. This makes it difficult to incorporate guest metal nanoparticles without compromising the 1 T phase support. To circumvent these issues, here we propose a p-block element (In-O) doping strategy to stabilize the 1 T phase MoS 2 by moderating the surface orbital steric effect and strengthening the internal chemical bonding, and thus for the epitaxial Ru nanocatalyst graft on the stabilized 1T-MoS 2 for Li | |O 2 batteries. The experimental and theoretical analyzes indicate that the In-O-MoS 2 @Ru enhances the O 2 dissociation and facilitates the adsorption of LiO 2 intermediates. This effect promotes the growth of weakly crystalline Li 2 O 2 films during oxygen reduction reaction, which can be more easily decomposed during the oxygen evolution reaction, thereby enhancing the bifunctional-catalytic kinetics. When employed at the positive electrode for non-aqueous Li | |O 2 batteries, In-O-MoS 2 @Ru shows an overpotential of 0.37 V and a cycling life of 284 cycles at 200 mA g −1 with a final discharge specific capacity of 1000 mAh g −1 at 25 °C.
研究领域:
材料科学
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电化学
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储能技术
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纳米技术
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催化
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PubMed
高影响因子
Catalysts
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2025
·Vol. 15
·期 6
·544
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IF 4
Tingting Hu,Baozeng Ren,Liang Zhao
Hydrogen peroxide (H2O2) is an important industrial chemical that is widely applied in many areas. The direct synthesis of H2O2from H2and O2has proved to be a green and economic pathway. Pd-based bimetallic catalysts, due to their superior catalytic performances in this reaction, have attracted intensive attention. Herein, Tetrakis(hydroxymethyl)phosphonium chloride (THPC) was adopted as the protective ligand to immobilize Pd-Au alloy nanoparticles onto activated carbon (AC). The varied Pd/Au molar ratios demonstrated homogeneously distributed Pd-Au nanoalloys with average particle sizes ranging from 3.51 to 5.75 nm. The optimal ratio was observed over the Pd3Au1/AC-THPC catalyst with a maximum H2O2productivity of 165 mol/(kgPd·h) and selectivity of 82.3% under ambient pressure. The relationship between the electronic structure and catalytic activity indicated Pd0was the active site, while the presence of Au inhibited H2O2degradation rate. This research could help in the design efficient bimetallic catalysts for the direct synthesis of H2O2.
研究领域:
化学
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催化材料科学
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高影响因子
Journal of the American Chemical Society
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2023
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IF 15
Shang Shi,Zhenzhen Shen,Shanshan Li,Qian Wang,Rui Wen,Bing Liu
The use of carbon materials in porous electrodes has impressive advantages. However, precisely tailoring the multilevel pore structure of carbon electrodes remains an unsolved challenge. Here, we report a highly efficient site-selective growth strategy to synthesize colloidal carbon rings by templating patchy droplets. Carbon rings are used for the direct fabrication of self-standing porous electrodes with hierarchical pores for lithium–oxygen batteries (LOBs). In situ atomic force microscopy reveals that during discharge the discharge products densely nucleate and grow on carbon rings, demonstrating that such rings are a very potential electrode material in LOBs. The hollow carbon ring electrode (HCRE) possesses micrometer-scale channels formed by random packing of rings and nanochannels consisting of ring-shaped hollow cavities connected by nanosized pores in the wall. Both channels contribute to ion transportation and gas diffusion, but the storage of the discharge products mainly lies in micrometer-scale channels, leading to a high discharge capacity of LOBs (20 658 mAh/g). Our work paves a new way to construct hierarchically porous electrodes for application in electrocatalysis and electrochemical energy storage.
研究领域:
材料科学
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电化学能源存储
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高影响因子
Materials Today Communications
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2025
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IF 4.5
Jiaqi Wang,Xiqiang Huang,Xingbao Zhu,Yuanguo Wu,Zining Man,Xiangyu Wen,Weiting Qi,Xing Tang,Zhe Lü
Despite their potential to enhance safety and design flexibility in next-generation lithium batteries, particularly lithium-oxygen (Li-O 2 ) systems, solid polymer electrolytes (SPEs) face persistent challenges of insufficient ionic conductivity and high interfacial resistance. To address these limitations, we developed a novel PEGDA-based quasi-solid-state electrolytes (QSEs) through in situ polymerization, strategically incorporating three functional additives: cellulose acetate (CA), N-methyl-2-pyrrolidone (NMP), and fluoroethylene carbonate (FEC). The electrolyte design leverages multiple synergistic mechanisms: hydrogen bonding between CA and NMP optimizes microstructural organization for efficient Li⁺ transport pathways; carbonyl groups in NMP coordinate with Li⁺ to facilitate LiTFSI dissociation, while oxygen-rich functional groups in CA provide supplementary Li⁺ coordination sites; FEC is introduced to further improve interfacial stability. This molecular engineering approach achieves an impressive room-temperature ionic conductivity of 8.54 × 10 −4 S cm −1 and a high lithium-ion transference number of 0.78. The QSE demonstrated excellent cycling stability (>900 h) in lithium symmetrical batteries and significantly improved the discharge capacity (12243 mAh g −1 ) and long-term cycling performance (590 h) of Li-O 2 batteries. These results highlight the efficacy of our multi-functional additive strategy in overcoming fundamental limitations in solid electrolytes, offering important insights for the rational design of high-performance energy storage systems.
研究领域:
储能
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材料科学
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电化学
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聚合物电解质
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电池技术
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高影响因子
Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Zehui Fan,Zhisen Li,Dan Mo,Jingyang Zhang,Shuyi Yang,Yun Li,Changlong Bi,Chong Peng,E Tao
Modulation of nano electrocatalysts for targeted excitation of different reactive oxygen species (ROS) is a key challenge to achieve environmentally catalyzed efficient pollutant degradation. In this study, multivalent copper catalysts (Cu (0)/Cu (I)/Cu (II)) load on the surface of biochar (CBX) are prepared by the hydrothermal-impregnation method, and the modulation effect of different valences of copper on the pathway of reactive oxygen species (ROS) generation is investigated. X-ray diffraction (XRD) analysis shows the coexistence of three copper valence states. Radical scavenging experiment and DFT calculations indicate that Cu (I) dominates the adsorption and activation of peroxodisulfate (PS) to efficiently generate ·SO 4 - and ·OH. Cu (II) selectively generates 1 O 2 by modulating the dissolve oxygen conversion pathway; whereas Cu (0) acts as an activation center for bound oxygen and significantly promotes ·O 2 - generation. The nano-electrocatalytic system prepared at 600°C (CB6-PS) degraded 98.3% of enrofloxacin (ENR) over a period of time (60 min). Mechanistic studies indicate that the catalytic system realizes the coupling reaction between the radical pathway (·SO 4 - /·OH /·O 2 - ) and the nonradical pathway ( 1 O 2 ) by the synergistic action of multivalent copper, which providing a new theoretical basis and technical strategy for the development of targeted ROS generation function.
研究领域:
环境催化
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材料化学
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污染控制
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纳米催化
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环境功能材料
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高级氧化技术
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Qiming Song,Zifan Li,Qun Peng,Xinwen Ou,Kun Zhao,Zhimin Dong,Liqun Ye,Chenchen Liu,Yunhai Liu,Jun He,Lai-Hon Chung,Bin Han
Photocatalytic O 2 activation, which produces miscellaneous reactive oxygen species (ROSs) via electron or energy transfer, is crucial for various chemical and biological processes. Unfortunately, controlling the exciton behaviors to flexibly regulate the generation of ROSs has rarely been explored and the underlying regulatory mechanisms remain poorly understood. Here, via linkage orientation engineering of covalent organic frameworks (COFs), we showcase a facile strategy for the flexible regulation between 1 O 2 and H 2 O 2 generation in photocatalytic O 2 activation. Imine-based COFs equipped with donor (D)-N=C-acceptor (A) chain (TFPT COFs) exerts effective H 2 O 2 production via electron transfer, while its structurally isomeric COFs with reversed imine orientation (TAPT COFs) tends to singlet oxygen ( 1 O 2 ) photosynthesis via energy transfer, attaining high efficiency for pollutant removal. Based on the results from ultrafast spectroscopy and theoretical calculations, when the N atom of the imine linkage is close to the electron acceptor, it diminishes the surface potential difference and increases the exciton binding energy; this favors the activation of the spin-triplet state excitons via an energy transfer process. Conversely, a strong built-in electric field is created when this N atom is adjacent to the electron donor, which encourages the dissociation of excitons into carriers and their subsequent separation.
研究领域:
化学
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材料科学
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生物学
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高影响因子
危险品化学品经营许可证（带存储）