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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APPLIED CATALYSIS B-ENVIRONMENTAL
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2026
·
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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JOURNAL OF HAZARDOUS MATERIALS
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2026
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IF 10.6
Fen Liu,Wei Xiang,Chen Wang,Yongchun Zhao,Tao Zhou,Mingjie Huang,Xiaohui Wu
High-concentration glyphosate (Gly) wastewater presents a formidable remediation challenge due to its recalcitrance and the inherent risk of generating toxic intermediates like aminomethylphosphonic acid (AMPA). Herein, we report a facile “waste-treats-waste” strategy utilizing a self-accelerated Fe(II)/O 2 system that operates efficiently under neutral pH, effectively circumventing the acidic constraints of traditional Fenton processes. This system achieved a 57% Gly removal efficiency (initial concentration 0.5 g/L) within 60 min, with a kinetic rate constant ( k obs = 0.029 min −1 ) significantly outperforming conventional oxidation technologies. Mechanistic investigations reveal that Gly acts as a suicide ligand, forming an inner-sphere Fe(II)-Gly complex that lowers the Gibbs free energy barrier, thereby rendering O 2 activation thermodynamically favorable. The degradation proceeds via a dual-pathway mechanism, synergizing hydroxyl radical (•OH) attack (∼40%) with a dominant intramolecular ligand-to-metal charge transfer (LMCT) process (∼60%). Crucially, density functional theory (DFT) calculations elucidate that Fe(III) coordination induces a regioselective weakening of the C–N bond adjacent to the phosphonate group. This steric and electronic modulation steers the reaction pathway toward the preferential formation of benign glycine, successfully suppressing the generation of highly toxic AMPA. Bioassays using Tetrahymena thermophila confirmed that this glycine-selective pathway optimization significantly mitigates the acute toxicity of the effluent, validating the system as a sustainable and eco-safe solution for herbicide wastewater treatment.
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高影响因子
Nature Communications
·
2026
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IF 18.1
Li Lei,Hua Minghao,Li Jiafeng,Guo Yun,Nie Yingjian,Zhang Boya,Hui Xiaobin,Zhang Luyuan,Zhang Zhiwei,Wang Rutao,Wang Chengxiang,Yin Longwei
Despite progress on noble-metal high-entropy alloy catalysts, noble-metal-free high-entropy alloy catalysts continue to face limitations in activity and stability. Atomic defect engineering holds promise for unlocking catalytic potential, yet efficient strategies for designing defects to simultaneously tailor electronic structures and enhance catalytic active sites in noble-metal-free high-entropy alloys remain challenging. Here, we report a general rule to drive twin formation via precisely tuning lattice strain in metallic nanomaterials. By modeling twin formation energy as a descriptor and employing a gradient-radius hetero-atomic doping strategy, we derive a generalized lattice strain-twin formation energy function that determines critical strain for twinning propensity. Guided by this principle, Ce is incorporated into CuCoNiMnMo nanoparticles, promoting coherent five-fold twinning along {111} planes. Twin boundaries generate high-activity sites by disrupting atomic symmetry and reducing coordination numbers, while modulating band width via altered orbital overlap. Meanwhile, strong Ce-O affinity forms an amorphous CeO x passivation layer on twinned noble-metal-free high-entropy alloy, triggering hetero-interfacial electron transfer. These effects synergistically optimize reaction kinetics. Consequently, the engineered catalyst achieves a 405-cycle lifespan in lithium–oxygen batteries and operates across −20 to 80 °C. Our study brings fundamental insights into defect engineering for electrocatalysis in energy conversion fields.
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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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高影响因子
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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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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Journal of Materials Chemistry C
·
2020
·Vol. 9
·期 5
·1593-1603
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IF 7.059
Guoming Gao,Ximeng Wang,Qifeng Chen,Caibo Xie,Jie Zheng,Huailin Fan,Lulu Ma,Ruifang Guan,Yanfen Fang,Xun Hu
Surface fluorinated TiO2 has received extensive attention in recent years due to the improved photocatalytic reactivity compared with that of pure TiO2. However, the synergy of surface fluorine (FS) and oxygen vacancy (VO) is not clear and needs further study. Here we systematically studied the effect of FS, VO and acidic sites of TiO2 nanosheets on the selective photocatalytic oxidation of benzylamine to imine. The photocatalytic activity first increased and then decreased as the content of FS decreased and VO increased. The photocatalytic activity reached a summit with the imine yield of 92.1% over TiO2-B-6 h, which is mainly due to the synergy between FS and adjacent VO, forming the frustrated Lewis pair that boosts the activation of O2. The varied contents of FS and VO not only cause an evident change in the amount of acidic sites, but also affect the band structure and separation efficiency of charge carriers. The experimental and calculation results demonstrate that the coexistence of FS and VO boosted the separation efficiency, density and mobility of photogenerated charge carriers, resulting in the improved photocatalytic activity. The improved photocatalytic activity can be attributed to the combined effects of FS, VO and acidic sites. This work provides a strategy for the explicit regulation of surface species on TiO2 nanosheets for improved photocatalytic activity.
研究领域:
材料科学
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环境科学
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化学工程
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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
Materials Today Communications
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2025
·
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
Chem
·
2019
·
IF 18.205
Rongan Shen,Wenxing Chen,Qing Peng,Siqi Lu,Lirong Zheng,Xing Cao,Yu Wang,Wei Zhu,Juntao Zhang,Zhongbin Zhuang,Chen Chen,Dingsheng Wang,Yadong Li
Summary The electrochemical direct synthesis of hydrogen peroxide (H 2 O 2 ) is significant but still challenging because of the lack of highly selective and active catalysts. Here, we report the synthesis of hollow nanospheres constructed by atomically dispersing platinum in amorphous CuS x support (h-Pt 1 -CuS x ) with a high concentration of single atomic Pt sites (24.8 at%), and this catalyst can consistently reduce O 2 into H 2 O 2 with selectivity of 92%–96% over a wide potential range of 0.05–0.7 V versus RHE in HClO 4 electrolyte. Scanning transmission electron microscopy and X-ray absorption fine structure spectroscopy confirmed the atomically isolated form of Pt with a low valance of +0.75. An electrochemical device that can synthesize H 2 O 2 directly from H 2 and O 2 is fabricated with H 2 O 2 productivity as high as 546 ± 30 mol kg cat − 1 h −1 . The well-defined and high-concentration single atomic Pt sites result in ultrahigh productivity of H 2 O 2 .
研究领域:
材料科学
·
电化学
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高影响因子
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