GREEN CHEMISTRY
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2025
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IF 9.2
Shuling Liu,Tongjun Li,Guozheng Dong,Xinao Wei,Keke Zhao,Bangan Lu,Yu Chen,Yanyan Liu,Jianchun Jiang,Baojun Li
To develop low-cost and efficient oxygen reduction reaction (ORR) electrocatalysts, single-atom catalysts (SACs) have attracted great attention to become vital to the applications of zinc-air batteries (ZABs) because of their high catalytic activity. The development of integrated SACs as self-supporting electrodes is crucial for ZABs to overcome the drawback of powder catalysts requiring binder. Herein, an integrated atomically dispersed FeSA/NC catalyst was obtained by pyrolysis of Fe-containing ZIF-8 on fir wood-derived carbon. The atomically dispersed Fe-N4 is an efficient catalytic active site for ORR. The self-supported ordered porous structure and continuous conductive network of the catalyst provide favorable conditions for the rapid mass/electron transfer. FeSA/NC catalyst demonstrates a positive half-wave potential of 0.90 V in 0.1 M KOH electrolyte and 0.80 V in acidic solution. The outstanding ORR activity outperforms those of commercial Pt/C and most reported M-N-C (M=Fe, Co, Ni, etc.) catalysts. A quasi-solid-state ZAB using the FeSA/NC in cathode shows an excellent peak power density of 77 mW cm–2 at 121 mA cm–2. The performance in quasi-solid-state batteries exceeds that of most other catalysts. This work provides a new path to the catalytically active carbon via design of self-supporting SACs, and a clear demonstration of prospects in quasi-solid-state energy devices.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2025
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IF 4.1
Xuanhao Zhang,Shanshan Wang,Zhanyu Ding,Haizhou Zhang,Xiaochun Ma,Xiaoming Zhou,Yu Ma,Yanlu Mu,Jiemei Yu,Taizhong Huang
Developing transition metal-based catalysts is a feasible approach to decrease the cost of fuel cells. In this paper, we synthesized a worm-like carbon nanotubes (CNTs) encapsulated Fe 3 P and Fe 0.8 Mn 0.2 alloy based catalysts (FP/FM@CNTs) for oxygen reduction reaction (ORR) by calcination method. The precursor for the calcination was prepared by hydrothermal method. The CNTs encapsulation structure was confirmed by SEM, HRTEM, XRD, XPS and EDS tests. The electrocatalytic performances for ORR of the catalyst were examined in 0.1 M KOH electrolyte by using CV, LSV, Tafel, EIS, RDE and RRDE tests. The obtained results presented that the half-wave potential(E 1/2 ) of FP/FM@CNTs catalyzed ORR was 0.892 V (vs. RHE), the maximum current intensity and the Tafel slope of FP/FM@CNTs catalyzed ORR were superior to that of the Pt/C catalyst. The density function theory calculation ascertained that the encapsulated Fe 3 P made the carbon atoms in surface layer CNT in negative electron state that could transfer electrons easily to oxygen molecular and promote the ORR happening. On the other hand, the CNTs encapsulation structure protected the Fe 0.8 Mn 0.2 alloy and Fe 3 P from the directly contact with electrolyte and other reactants, which assured the long-term operational stability of the catalysts. The content of this paper presents a novel approach for designing high-performance catalysts.
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ACS Applied Energy Materials
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2025
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IF 5.5
Na Jin,Xiao Yang,Yong Li,Wanjing Lai,Hailin Jiang,Yanghua Li,Kuo Liu,Yimeng Cai,Linjie Zhang,Lili Han
Hydrogen, characterized by its high energy density, efficiency, and environmentally benign output, emerges as a promising alternative to fossil fuels. However, the development of robust hydrogen oxidation reaction (HOR) catalysts for efficient energy conversion remains a significant challenge. Herein, a NiRu nanoalloy catalyst supported on N-doped hollow carbon nanocages (NiRu/NC) is synthesized via a tandem pyrolysis method. The NiRu/NC catalyst exhibits superior alkaline HOR activity, achieving diffusion-limited current density of 2.56 mA cm–2 and maintaining stability for 80,000 s with a decay rate of only 5.9%, compared to a 28.7% decay rate for benchmark Pt/C after 35,000 s. Additionally, it demonstrates remarkable resistance to CO poisoning, with the current density decreasing by only 50.7% after 1800 s, while the current density of Pt/C dropped to 0 after 800 s. Density functional theory calculations indicate that Ni in the NiRu nanoalloy effectively modulates the electron distribution, thereby ameliorating the electronic structure and enhancing the adsorption of reaction intermediates. These optimizations endow NiRu/NC with both favorable hydrogen-binding energy (HBE) and hydroxyl-binding energy (OHBE), leading to improved HOR efficiency. This work not only offers an innovative approach for synthesizing high-performance alloy-based HOR catalysts but also deepens the fundamental understanding of the bimetallic synergistic mechanisms in HOR catalysis.
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Nature Communications
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2025
·Vol. 16
·期 1
·1-13
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IF 15.7
Tao Xiwen,Hou Li,Wang Xinyi,Jin Jing,Li Huana,Gao Faming
Conjointly activating metal and oxygen sites to trigger the adsorbate evolution and lattice oxygen mechanisms coupled path holds promise for balancing activity and stability in oxygen evolution reaction catalysts, yet confronting great challenges. Herein, we develop Fe species and oxygen vacancies co-regulated Ni-(oxy)hydroxide from the deep reconstruction of Fe-Ni 2 P/NiMoO 4 pre-catalyst achieving the adsorbate evolution and lattice oxygen dual-path mechanism. Experimental details and theoretical calculation analysis reveal the enhanced adsorbate evolution mechanism kinetics at the Ni sites via the co-regulation of Fe species and oxygen vacancies, while the Fe incorporation activates the O sites with preferable adsorption free energy for lattice oxygen mechanism intermediates. Benefiting from the dual-path mechanism, the activated catalyst affords an ampere-scale current density of 1.0 A cm -2 at low overpotentials of 274.5 ± 4.2 and 299.1 ± 2.8 mV in alkaline freshwater and seawater, respectively, and maintains seawater electrocatalysis for 500 h in the anion exchange membrane water electrolysis. This work demonstrates a strategy to trigger the coupled mechanism for efficient and stable electrocatalytic water splitting under harsh conditions.
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PubMed
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JOURNAL OF POWER SOURCES
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2025
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IF 7.9
Lin Wu,Chunyu Ji,Xueyan Li,Zirui Liu,Hao Yang,Feng Qiu,Zhili Peng,Qingju Liu,Longzhou Zhang
Despite heteroatom doping is a smart approach to facilitate the oxygen reduction reaction (ORR) performances of nanocarbon catalysts, two dominant issues still retain as significant obstacles. One is the relatively low activity compared to benchmark catalysts, the other is the ambiguous elucidation of the catalytic mechanism for dual heteroatom-doped catalysts. Here, nitrogen and sulfur co-doped carbon-dots electrocatalyst (HT-CDs) are simply prepared by means of physical activation with water vapor on the carbon-dots precursor. The material exhibits excellent ORR performance under alkaline conditions, achieving a half-wave potential of 0.91 V (vs RHE), surpassing most metal-free catalysts and Pt/C. Further theoretical studies reveal that N/C-S-N structure fills more electrons in the anti-bond orbitals that promoting the charge transfer from the catalyst to the reactant O 2 , thus enhancing the efficient ORR process.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2025
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IF 8.3
Biye Niu,Feixiang Gao,Zekun Jing,Taiping Fu,Yufeng Liu,Yakun Guo,Maobing Shuai
In confined environments, hydrogen accumulation presents significant safety hazards, necessitating the development of efficient hydrogen uptake materials. Conventional Pd/C-DEB hydrogen getter is severely compromised by CO poisoning. This study introduces a one-step mechanochemical ball milling approach that integrates Pd/C catalysts with DEB to fabricate a CO-tolerant hydrogen getter. A DEB conversion rate of 75.2 % is achieved under an H 2 atmosphere containing 1 % CO, representing a sixfold improvement over the untreated sample. Ball milling refines Pd nanoparticles, increases surface area, generates multiscale defects, strengthens metal-support interactions, enhances electron transfer, modulates the Pd d-band structure, and reduces CO adsorption energy, thereby exposing more active sites for hydrogen uptake. This approach is also applicable to Pt/C, Rh/C, and other platinum-group metal systems, providing a versatile strategy for designing durable and CO-resistant getters in energy storage and conversion technologies.
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ACS Catalysis
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2025
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IF 13.1
Luyao Ge,Heng Liang,Wei Lan,Maodi Wang,Xiaoming Zhang,Aiping Jia,Xiang-Kui Gu,Qihua Yang,Xiaobo Li
Enzyme cofactor-mediated biochemical cascades in living cells showcase nature’s capacity for efficient, selective multistep transformations, inspiring artificial chemoenzymatic systems that merge enzymatic specificity with the versatility of synthetic catalysts via the cofactor. Practical implementation of such systems is, however, constrained by poor selectivity, enzyme incompatibility, and limited turnover in nonenzymatic in situ cofactor regeneration. Here, molecular ligand-directed interfacial tailoring of supported Pt catalysts is shown to overcome these challenges, achieving >99% regioselective NADH regeneration from NAD+ with H2 as a clean reductant, while enhancing the activity and stability. Machine learning-guided analysis of a structurally diverse ligand library, validated experimentally, identifies the surface Pt2+ fraction as a robust, predictive electronic descriptor for selectivity classification across catalyst variants. Integration of the ligand-optimized catalyst with an NADH-dependent dehydrogenase delivers asymmetric hydrogenations with >99% enantiomeric excess and benchmark in situ NADH turnover numbers. This study demonstrates an H2-driven chemoenzymatic platform that bridges heterogeneous metal catalysis and enzymatic catalysis, offering immediate relevance to a wide range of applications, including fine chemical synthesis and artificial photosynthesis.
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Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Haoyang Huang,Yanxiao Si,Jiajun Zou,Jiawei Li,Yongjie Li,Wenxin Huo,Haichuan Zhang,Yingjie Li,Ji Li
The H*-mediated electro-Fenton system, a novel byproduct-free H 2 O 2 activation technology, faces economic and universality challenges. This study fabricated a non-noble nickel-based catalyst to replace palladium (Pd), constructing a sandwich-structured NiO/oxidized carbon black electrode (SE-NiO/OCB) enriched with three-phase interfaces (TPI) for tetracycline (TC) removal. SE-NiO/OCB demonstrated efficient catalysis of atomic H* generation, achieving a significantly higher ·OH exposure of 19.18 × 10 −12 M·s compared to SE-OCB (5.37 × 10 −12 M·s). Additionally, the SE-NiO/OCB exhibited a remarkable TC removal efficiency of 96.7 % within 90 min, far exceeding SE-OCB (55.9 %). By leveraging H + /H 2 O as H* sources, the SE-NiO/OCB maintained ≥ 83.4 % TC removal across a broad pH range of 3–11, validating exceptional pH adaptability. Additionally, SE-NiO/OCB achieved a removal rate of ≥ 86.7 % for multiple tetracycline antibiotics at neutral pH, underscoring its broad applicability. The cost of utilizing SE-NiO/OCB to drive the H*-mediated E-Fenton reaction for TC removal was merely 0.05 RMB/(mg TC), which was significantly lower than that of noble metal catalysts. Thus, this work resolved critical economic and universality limitations in H*-mediated electro-Fenton processes, advancing scalable antibiotic wastewater treatment strategies.
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Inorganic Chemistry Frontiers
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2025
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IF 6.4
Lijia Zhou,Xiangjiang Dong,Qiang Li,Xianran Xing
We systematically investigated the superconducting properties of 2H-PtxTaS2 (0 ≤ x ≤ 0.08). As the platinum (Pt) content increases, the charge density wave (CDW) in 2H-TaS2, which appears at approximately 75 K, is progressively suppressed and completely disappears in Pt0.06TaS2. Meanwhile, the superconducting transition temperature (Tc) first increases and then decreases, reaching its maximum value of approximately 4.85 K at x = 0.06. This phenomenon suggests a competitive interplay between CDW and superconductivity (SC) in this system. Further measurements of the superconducting parameters of Pt0.06TaS2 indicate that the enhancement of Tc is primarily attributed to an increase in the density of states at the Fermi level.
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ChemCatChem
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2025
·
IF 3.9
Tianjiao Ling,Fan Lv,Ruiqi Guo,Yi Cao,Mingzhi Zhang,Huihua Wang,JinXin Chen,Huaqing Li,Hao Ren,Guangcheng Li,Hongwei Li,Minqi Sheng
The design of bifunctional catalytic electrodes with high performance and low cost is the key to improving hydrogen production efficiency by water splitting. However, achieving the coexistence of high activity and stability of catalytic materials still faces challenges. Herein, we designed and prepared a self-supported electrode material (Ni₂P/NiSe@CNTs/CC) through the combined action of metal-catalyzed carbon nanotube (CNTs) growth, selenization, and phosphating. In this process, CNTs are grown in situ on the carbon cloth (CC) surface, and the inner cavity is filled with heterogeneous Ni₂P/NiSe nanoparticles. The optimized Ni₂P/NiSe@CNTs/CC electrode demonstrates an overpotential of 116.2 mV at -10 mA cm-² for hydrogen evolution reaction (HER) and 332.4 mV at 50 mA cm-² for oxygen evolution reaction (OER) in 1.0 M KOH electrolyte, respectively. Accordingly, the Ni₂P/NiSe@CNTs/CC||Ni₂P/NiSe@CNTs/CC couple achieves efficient water splitting with a cell voltage of 1.67 V at 10 mA cm-² and 2.01 V at 50 mA cm-², respectively. Moreover, Ni₂P/NiSe@CNTs/CC||Ni₂P/NiSe@CNTs/CC couple only decays by 0.5% after 100 hours of continuous operation at 10 mA cm-², indicating that it has considerable stability. Dynamic bubble monitoring results display that the Ni₂P/NiSe@CNTs/CC electrode/ electrolyte interface has a strong bubble escape capability, which promotes the cyclic service of the catalytic active sites.
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Yu-Xuan Fu,Shu-Yi Huang,Ming-Shuai Sun,Yan Zhou,Dan-Dan Cai,Wen-Shuai Zhu,Wei Hui,Duan-Jian Tao
Current industrial catalysts for α-pinene hydrogenation suffer from harsh reaction conditions and poor selectivity to cis -pinane, primarily due to their inability to effectively adsorb α-pinene in a specific favorable configuration on the catalyst surface. In this study, a high-specific-surface-area, rod-shaped CeO 2 -supported ultra-fine Ru nanoparticle (average particle size of 4 nm) catalyst was synthesized via hydrothermal method for the highly stereoselective hydrogenation of α-pinene to cis -pinane. The resulting Ru/CeO 2 -H catalyst achieved an α-pinene conversion of 99.3 % and an impressive cis -pinane selectivity of up to 99.6 % under exceptionally low temperature (30°C), 0.6 MPa H 2 and 0.5 h with high TOF (1236 h −1 ). Density functional theory (DFT) calculations indicated that α-pinene preferentially adsorbs onto the Ru surface via the backside of its intramolecular dimethyl bridge. This particular adsorption mode lowers the energy barriers for further hydrogenation to generate cis -pinane. The oriented dimethyl-up configuration of α-pinene and ultra-low activation energy (12.04 kJ/mol obtained from kinetic tests) enable the highly selective production of cis -pinane at ambient temperature. Furthermore, the strong interaction between the CeO 2 -H support and highly dispersed Ru, combined with the ambient-temperature reaction conditions, effectively prevents metal nanoparticle agglomeration and coking, imparting the catalyst with exceptional stability. Notably, the catalyst was reused at least 15 times without observing any significant deactivation, demonstrating its significant potential for practical applications.
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JOM
·
2025
·
IF 2.3
Zhao Yingqing,Deng Yifan,Liu Jieqiang,Li Min,Li Ying
Sodium-ion batteries (SIBs) are usually considered as a promising alternative to lithium-ion batteries due to the abundant resources of sodium. Antimony has been widely used for SIBs anodes because of its high capacity, which often suffers the issue of unstable structure, leading to a poor performance and unstable solid electrolyte interface (SEI). In order to improve the stability of anodes, the electrochemical reduction of solid antimony sulfide/carbon nanotubes (Sb 2 S 3 /CNTs) to a antimony/carbon nanotubes (Sb/CNTs) composite used as an anode for SIBs using deep eutectic solvent is reported for the first time. The electrolytic Sb particles will be wrapped by the CNTs after the electrochemical desulfurization approach, resulting in an improvement of the stability of the electrolytic products used for anodes. The electrolytic Sb/0.5CNTs anode exhibits a high specific capacity of 612.3 mAh g −1 after 200 cycles at a current density of 0.1 A g −1 , and a high specific capacity of 480.9 mAh g −1 after 150 cycles at a current density of 0.5 A g −1 . The results demonstrate the feasibility of the direct electrochemical desulfurization strategy from solid sulfides and provide a novel route for producing SIBs anodes.
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