ChemCatChem
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2025
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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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Journal of Energy Chemistry
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2025
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IF 14.9
Lun Li,Di Liu,Zhichao Yu,Youpeng Cao,Chengcheng Zhong,Chunfa Liu,Jiao Yang,Wendi Zhang,Weng Fai Ip,Hui Pan
The incorporation of high-valence metals into FeCoNi-based oxide/hydroxide/oxyhydroxide matrices is widely acknowledged as an effective approach to enhance oxygen evolution reaction (OER) performance. Traditionally, it is assumed that these metals could maintain structural stability during operation. Here, our in-situ and ex-situ characterizations reveal that the dynamic electro-dissolution behavior of Mo 6+ and W 6+ species in FeCoNiMoW pre-catalyst leads to fast formation of catalytic-active (Mo, W) co-incorporated metal oxyhydroxides, which play a key role in the OER performance. This leaching process enables structural reconstruction, while concurrently optimizing the adsorption of the oxygen intermediate. The resulting catalyst exhibits exceptional OER activity, achieving an overpotential of 218 mV at 10 mA cm −2 , as well as remarkable stability with a degradation rate of only 8.7 μV h −1 over 720 h at 500 mA cm −2 . Furthermore, anion-exchange membrane water electrolyzers based on FeCoNiMoW//Pt/C can stably operate at 500 and 1000 mA cm −2 with low cell voltages of 1.70 and 1.84 V, respectively. The cost of the electric bill using this catalyst is notably low, at only $0.88 per kg, which is significantly below target of $2.00 per kg set by the U.S. Office of Clean Energy (OCE) for 2026. These findings offer valuable insights into the critical role of high-valence metals in advancing the OER process and underscore the substantial potential of this approach for industrial scale-up applications.
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Fundamental Research
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2025
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IF 6.3
Zhong Wang,Tuo Zang,Ye Ziyu,Siyuan Zhang,Guojian Li,Xiaoming Liu,Qiang Wang,Shuang Yuan
Precise anchoring and high-density utilization of platinum single atoms (Pt SA ) remain critical challenges in advancing efficient hydrogen production via water electrolysis. Here, we present an innovative magnetic-field-assisted electrodeposition strategy for the controllable synthesis of high-density Pt SA on two-dimensional MXene substrates. Application of a 0.6 T magnetic field significantly enhanced Pt SA deposition kinetics, yielding a 2.1-fold increase in the deposition rate. Numerical simulations confirmed that magnetohydrodynamic (MHD) effects induced by the magnetic field were the primary mechanism driving this enhanced deposition efficiency. The optimized Pt SA -0.6@MXene/NF catalyst exhibited outstanding hydrogen evolution reaction (HER) performance in 1 M KOH, achieving an ultralow overpotential of 12 mV at 10 mA cm −2 , along with a Tafel slope of 29 mV dec −1 . Notably, the catalyst demonstrated 66.1-fold higher Pt mass activity (3458.7 A g −1 ) compared to commercial Pt/C (52.3 A g −1 ) at a 50 mV overpotential. Density functional theory (DFT) calculations revealed that the high-density Pt SA configuration synergistically enhances MXene's electrical conductivity while lowering the d-band center, thereby optimizing the energy barrier for hydrogen intermediate (H*) adsorption. This work provides a novel strategy for regulating the magnetic-field-assisted deposition of Pt SA catalysts, offering a new avenue for designing high-performance water electrolysis catalysts.
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EUROPEAN POLYMER JOURNAL
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2025
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IF 6.3
Jie Liu,Jun Yang,Zijia Zhang,Qian Jiang,Lele Sun,Chaoyi Peng,Jin Wang,Li Xiang,Anlian Pan
In order to prepare polyimide materials with excellent optical transparency and UV barrier, the effects of the number and substitution position of −CF 3 groups on polyimide properties were investigated. Researchers synthesized four novel diamine monomers (BPA-O, BPA-NH 2 , BPAF-O, BPAF-NH 2 ) and synthesized eight high-performance colorless polyimides (PI-1 ∼ PI-8). On the one hand, the strong electron-withdrawing effect of −CF 3 restricts electron movement within the molecular chain, weakening the CTC effect of the molecular chain and thereby enhancing the transparency of the film. On the other hand, the ortho -substitution of −CF 3 on the imide ring induces greater twisting of molecular chains, disrupts their close packing, and thereby exerts a positive effect on enhancing the optical transparency of the film. The high bond energy of the C-F bond and the introduction of the flexible group −O- act as an “energy buffer,” suppressing UV-induced main chain breakage and achieving high UV barrier. All CPI films exhibit excellent transparency and thermal stability, with a cut-off wavelength range of 325 nm-381 nm and a transmittance range of 78.7 %-88 % at 550 nm. They have good optical properties, with T d5% distributed in the range of 511.5 °C − 533.7 °C, and the glass transition temperature ( T g ) distributed in the range of 197.3 °C-234.4 °C, demonstrating good thermal stability. Additionally, the cut-off wavelength is at a relatively high level, reaching up to 381 nm.
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Research
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2025
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IF 10.7
Ziliang Yuan,Yijing Gao,Qingjie Tang,Jianguo Wang,Xun Li,Zehui Zhang
Organonitrogen chemicals with C=N bonds are one of the most important groups of chemicals with broad applications, but their synthesis via reductive coupling remains a great challenge, because of the favorable hydrogenation of C=N bonds into C–N bonds. In this study, a nitrogen-doped carbon-supported β-MoO 3 catalyst with abundant oxygen vacancies (O v ) was discovered to be robust in the reductive coupling of nitro compounds with biomass-derived alcohols toward the synthesis of organonitrogen chemicals, including imines and N -heterocycles with C=N bonds. The O v in β-MoO 3 serves a crucial role in the adsorption and activation of substrates via the electronic interaction between the negatively charged oxygen atoms in these substrates and the O v sites in β-MoO 3 . The presence of O v greatly lowers the energy barriers of the reductive coupling reaction, and the electron transfer from alcohols to nitro compounds is mediated by the Mo 5+ /Mo 6+ redox cycle. Our method demonstrates excellent selectivity to C=N bonds and is effective for a wide substrate scope including the highly inert methanol and ethanol. This study highlights the use of non-noble metal oxides as alternatives to traditional metal nanoparticles for various challenging organic transformations.
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PubMed
高影响因子
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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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 MATERIALS SCIENCE & TECHNOLOGY
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2025
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IF 14.3
Linyin Huang,Xinyue Wei,Yuan Yu,Dongfeng Sun,Yanning Qu,Jianlong Wen,Xiaoya Yuan,Qingmei Su,Fangyou Meng,Gaohui Du,Youqing Wang,Bingshe Xu,Kai Wang
In NiP-based catalysts, although Ni 2 P and Ni 5 P 4 have relatively high catalytic activity, the catalytic performance of single-phase Ni 2 P or Ni 5 P 4 is still far from that of noble metal catalysts. The dual-phase heterojunction has better catalytic performance than single-phase materials due to its faster interface charge transfer rate and more active sites. The Ni 2 P/Ni 5 P 4 @CC heterostructural catalyst with oriented porous nanosheet arrays grown on carbon cloth (CC), was in-situ constructed through the controllable phase transition of Ni 2 P. By modulating the amount of P source (P-dependent) or the phosphating reaction time (Time-dependent), the degree of the Ni 2 P phase transition could be modulated, thus obtaining the Ni 2 P/Ni 5 P 4 @CC heterostructural catalyst with the required component ratio of Ni 2 P and Ni 5 P 4 . When the ratio of Ni 2 P and Ni 5 P 4 was 15.7:84.3, the Ni 2 P/Ni 5 P 4 @CC catalyst had the best catalytic performance. Its hydrogen evolution reaction (HER) overpotentials were only 139 and 87 mV overpotentials reaching −10 mA/cm 2 in 1 mol/L KOH and 0.5 mol/L H 2 SO 4 , respectively, which was much lower than that of the single-phase Ni 2 P@CC (base: 278 mV; acid: 123 mV) and Ni 5 P 4 @CC (base: 166 mV; acid: 106 mV) catalysts. Specially, in acidic electrolyte, HER overpotential at a higher current density of −100 mA/cm 2 of the Ni 2 P/Ni 5 P 4 @CC catalyst was 270 mV, which was even lower than that of the Pt/C catalyst (328 mV), indicating that the Ni 2 P/Ni 5 P 4 @CC heterostructural catalysts had promising prospects for commercial applications. The mechanism of catalytic performance enhancement was investigated by the density functional theory (DFT) calculations.
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NEW JOURNAL OF CHEMISTRY
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2025
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IF 2.5
Liang Xian,Shu Xin Liu,Jing Ma,Xiao Xia Tian,Wei Li,Zhao Min Liu
C60 has a spatial confinement effect as a carrier for Pt nanoparticles. In this paper, highly dispersed and uniformly sized ultrafine Pt nanoparticles (Pt/C60-A) were synthesized by a photoinduced method using green ascorbic acid as an auxiliary reducing agent in the presence of C60 space-confined. It was found that the morphology of Pt nanoparticles could be modulated by adjusting the wavelength of light (395 nm UV and 450 nm blue-violet, 650 nm red). Changing the concentration of the auxiliary reducing agent regulated the Pt nanoparticle loading and dispersion. In addition, an electron-rich surface is formed on the surface of Pt nanoparticles synthesized under strong metal-support interaction (SMSI). In the methanol oxidation reaction, the catalyst (Pt/C60-A3) prepared by 3 mL of 180 mM reductant, synergistically irradiated with blue-violet light (450 nm), showed catalytic activity and durability that were significantly better than those of commercial Pt/C catalysts. The catalytic performance of Pt/C60-A3 was unchanged before and after the durability test and showed high durability. In addition, Pt/C60-A3 also exhibits high catalytic activity and durability in the reduction of p-nitrophenol (4-NP), with an apparent rate constant (k) of up to 0.54 min-1, and the catalytic activity is still maintained at about 87% after seven cycles of the 4-NP reaction. This study provides a new insight and method for synthesizing and applying noble metal nanoparticles.
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Small
·
2025
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IF 12.1
Xinyu Cao,Liancen Li,Guangfu Qian,Qizhi Xie,Yuxuan Xie,Jiawei Li,Yunpeng Wang,Minsheng Lu,Jinli Chen,Panagiotis Tsiakaras
Developing efficient pH-universal hydrogen evolution electrocatalysts is critically needed yet challenged by pH-dependent. Here, a lignin-derived carbon-supported Ni/Cu/MoO 2 heterostructure (Ni/Cu/MoO 2 @LC) through multiphase interfaces design is engineered, which displays excellent electrochemical activity, featuring low potentials of −14.4/−201.5 (acidic), −44.5/−615.7 (neutral), and −28.2/−242.3 mV (alkaline) at −10/−1000 mA cm −2 . Theoretical and experimental analysis show that the Ni/Cu/MoO 2 @LC multiphase interfaces produce a synergistic coupling of compressive-tensile strains and interfacial electron transfer effect. This synergistic effect triggers electron redistribution, tailors the electronic configuration through d -band center optimization, and balances intermediate adsorption/desorption energetics. Additionally, lignin-derived carbon self-supported micro-nano-array structure enhances gas-liquid transport and corrosion resistance, allowing Ni/Cu/MoO 2 @LC to operate stably for at least 120 h, at −500 mA cm −2 in various pH solutions. Thus, this study provides a new idea for the design of cost-effective pH-universal HER electrocatalysts and a new approach for applying lignin-derived carbon in electrocatalysis.
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PubMed
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ACS Catalysis
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2025
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IF 13.1
Xiaoxiao Duan,Ning Wen,Shu Liu,Haiping Li,Xiuling Jiao,Dairong Chen,Yuguo Xia
Developing efficient and durable electrocatalysts for PEMWE is essential for advanced hydrogen production. Here, we introduce a lattice strain manipulation strategy through multiphase interface engineering, demonstrating its effectiveness in enhancing water-splitting efficiency while mitigating Ru dissolution in acidic environments. Specifically, an in situ combustion method is employed to synthesize the Ru-based hybrid (Ru/RuS2/RuO2), increasing the density of crystal boundaries and optimizing the lattice strain within the Ru/RuS2/RuO2 structure. The two-electrode system consisting of the bifunctional Ru/RuS2/RuO2 hybrid exhibits superior overall water-splitting performance (19 mV@10 mA cm–2 for HER and 177 mV@10 mA cm–2 for OER), achieving an impressive low cell voltage of 1.468 V at a current density of 10 mA cm–2 with only 14 ppb of Ru ion dissolution even after 500 h. Experimental analyses and theoretical calculations highlight the critical role of the multiphase interfaces in modulating electronic structures, enhancing hydrophilicity, and accelerating water-splitting reactions. Density functional theory calculations further reveal reduced energy barriers and increased Ru dissociation energy, attributed to the shortened Ru–O/Ru–S bonds as well as the decreased bonding band energy of these interactions. This work underscores the transformative potential of multiphase interface engineering in overcoming durability and efficiency challenges for Ru-based electrocatalysts.
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