CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Yirui Wang,Liuping Liang,Yuqing Tang,Wanling Xiao,Tao Zhou,Peikang Shen,Panagiotis Tsiakaras
Surface reconstruction is the key to improving the intrinsic activity of non-precious metal-based catalysts for the urea oxidation reaction (UOR). In this work, Cerium doped Nickel phosphide (Ce-Ni 5 P 4 ) porous nanosheets were synthesized by conventional hydrothermal and phosphorylation methods. It is found that the introduction of Ce 4f induces the electron transfer from P and Ni to Ce, increasing the chemical state of Ni, boosting the reconstruction of Ni 5 P 4 toward active substances of NiOOH with higher UOR activity and improves the UOR intermediates adsorption behavior on the (210) crystal plane for efficient electrochemical reaction. The results show that Ce-doped Ni 5 P 4 improves the UOR performance of only 1.33 V at 500 mA cm −2 , and exhibits exceptional stability over 120 h. Meanwhile, the AEMWE assembly by Ce-doped Ni 5 P 4 || MoNi foam possess a lower voltage of 2.37 V than RuO 2 ||MoNi foam at 1 A cm −2 , demonstrating an excellent performance in industrial applications. The in-situ Raman confirms the enhanced electrochemical reconstruction process caused by the introduction of Ce, which promotes the large current density UOR process. The theoretical calculations show that the stable (210) crystal plane without reconstruction is activated by the Ce doping, and the modulated electron distribution around the Ni sites weakens the binding energy of the Ni N bond, reducing the energy barrier of the rate-determining step for more efficient reaction kinetics. This work provides a hierarchical reconstruction strategy to promote the coupling of activated structures and stable bulks, improving the catalytic UOR activity at large current density and providing new insights for the development of catalysts for industrial applications.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-13
·
IF 15.7
Shen Huasen,Li Zhaohuai,Li Jiantao,He Qiu,Li Mengjun,Tian Yunan,Wu Guoning,Zhao Yan,Zhang Xuanxuan,Xiao Jingjing,Amine Khalil,Li Yuyu,Xie Ming,Lu Jun
The growth of lithium (Li) dendrites and the accumulation of dead Li (i.e., Li metal regions which are electronically disconnected from the current collector) significantly undermine the safety and performance of Li metal batteries. This study employs kilogram–scale atomic layer deposition technology to construct zinc oxide with a preferential (002) crystal orientation, which homogeneously forms on commercial carbon nanotube papers. Our approach emphasizes the importance of achieving a moderate Li adsorption energy and low Li migration energy barriers to suppress Li dendrite growth. In this work, we introduce the concept of “catalytic” effect for dead Li reconversion, as validated through time–of–flight secondary ion mass spectrometry, leading to a Li plating/stripping efficiency of 99.89%. The Ah–level Li metal pouch cells with high–nickel positive electrodes achieve a specific energy of 380 Wh kg −1 (based on the mass of the whole pouch cell) and demonstrate stable cycling under demanding conditions. Analysis of the cycled pouch cells confirms the structural integrity and provides insights into the mechanism of the dead Li “catalytic” conversion.
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Nature Communications
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2025
·Vol. 16
·期 1
·1-12
·
IF 15.7
Gao Xiaoyue,Ben Teng
Chiral drugs are essential in modern medicine, but separating their enantiomers is challenging due to their similar physicochemical properties. However, traditional methods are often costly and inefficient. Here we show that chiral covalent organic framework (CCOF-300) membranes, induced by chiral dopants (L-( + )-/D-(–)-tartaric acid), can achieve high enantioselectivity in separating chiral drugs. Specifically, CCOF-300 membrane achieved 100% enantiomeric excess in separating racemic N-Fmoc-N’-[1-(4,4-Dimethyl–2,6-dioxocyclohexylidene)ethyl]-lysine (Fmoc-Lys(Dde)-OH). We found that size matching and differences in diffusion rates between enantiomers are key factors in chiral separation. Additionally, there were no significant differences in the binding energy between ibuprofen (IBU), Fmoc-Lys(Dde)-OH, and CCOF-300, indicating that binding energy is not the dominant factor in chiral separation. This study proposes a cost-effective and scalable method for chiral drug separation, highlighting the potential of chiral induction strategy in improving chiral separation technology in the pharmaceutical industry.
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APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Shaobo Huang,Fanhui Meng,Zexin Liang,Mengqi Li
The pursuit of sustainable hydrogen production via water electrolysis urgently demands electrocatalysts reconciling industrial-grade activity, durability, and cost-effectiveness for the hydrogen evolution reaction. While transition metal selenides (TMSs) offer noble-metal alternatives with tunable electronic structures, monophasic variants suffer from compromised charge transfer kinetics, limited active site exposure, and cathodic degradation. Herein, we propose selenium anion electric field engineering via molybdenum ions regulated heterointerface construction in Ni 3 Se 4 /MoSe 2 heterojunctions anchored on nickel foam (denoted as Ni 3 Se 4 /MoSe 2 @NF). Multiscale mechanistic studies reveal that the reconstructed built-in electric field around the selenium anions in MoSe 2 demonstrates a lower hydrogen adsorption free energy (ΔG H* = 0.166 eV) via d-band center, with accelerating interfacial charge transfer. The resultant catalyst achieves an ultralow overpotential of 60 mV at 10 mA cm −2 (η 10 ) with a Tafel slope of 65.17 mV dec −1 . Particularly noteworthy is its industrial-grade stability, which exhibits only a 20 mV (η 100 ) increase after 200 h of continuous operation in 1 M KOH, coupled with near-unity Faradaic efficiency (over 98 %). This work establishes a heterointerface microenvironment regulation paradigm to break the activity-stability trade-off, providing a universal design principle for durable, high-flux water electrolysis.
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Nature Communications
·
2025
·Vol. 16
·期 1
·10766
·
IF 15.7
Zhang Jia,Guo Lu-Yao,Lin Xiao-Qian,Wen Gui-Hua,Zhang Xue-Feng,Yu Li-Hong,He Mei-Qian,He Yu-Mei,Zou Long,Zhang Meng-Tian,Cao Li-Ming,He Chun-Ting
Developing efficient chemical modification technologies for upgrading classic non-noble metal based electrocatalysts to further meet the demands of practical water electrolysis industry is of vital challenge. Here, we propose an organic-inorganic dual-modulation strategy to construct a cobalt hydroxide-based electrocatalyst, MEC-17, synthesized by an eco-friendly and facile microbial-mediated vulcanization method. This electrocatalyst, modified with both 2-methylimidazole and inorganic sulfur exhibits notable oxygen evolution reaction performance, achieving an overpotential of 285.6 ± 1.7 mV and exceeding 300 h of durability at a high current density of 1000 mA cm −2 . The operando characterizations and theoretical calculations reveal that sulfur dopant primarily shortens the Co−Co distances to support oxide path mechanism, while 2-methylimidazole plays a more critical role by modulating the d -band center of the Co sites, which optimizes intermediate adsorption for ensuring efficient O−O coupling. This work offers insights into the design of organic-inorganic hybrid electrocatalysts and contributes to understanding the origin of their electrocatalytic activities.
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CHEMISTRY-A EUROPEAN JOURNAL
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2025
·
IF 3.7
Jun Shen,Changhui Liang,Yuxin Zhang,Xiaoqiang Zhang,Huixiang Li,Yongxin Li,Songhai Xie,Z. Conrad Zhang
Bioethanol and furanics are currently prevailing additives to fossil-based transportation fuels. With the objective to lift the longstanding limitations of these biofuel additives, this work reports for the first time the synthesis of 2-ethoxy-2-methyltetrahydrofuran (2-EO-2-MTHF) as a co-upgraded fuel by reacting ethanol with 2-methylfuran (2-MF). The formation of 2-EO-2-MTHF is achieved through ethanol ethoxylation of 2-MF, enabled by a reverse Ni(OH) x /Ni catalyst under hydrogen pressure. Nickel hydroxide species over the Ni nanoparticles play a crucial role in activating ethanol and polarizing the partially hydrogenated dihydrofuran intermediates, favorably steering the reaction selectively toward the ethoxylation product. The reaction conditions, including pressure and temperature, are systematically optimized to enhance the yield of 2-EO-2-MTHF, and provide a means to beneficially tune the fuel compositions consisting mainly of 2-EO-2-MTHF and 2-MTHF, both are high energy density molecules. Importantly, the reverse Ni(OH) x -Ni catalyst allows a one-pot process to accomplish consecutive partial hydrogenation of 2-MF and ethanol ethoxylation. This work provides a practical strategy for upgrading biomass-derived polar primary fuel molecules into more versatile fuels and chemicals.
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Journal of Magnesium and Alloys
·
2025
·
IF 13.8
Shusheng Cao,Yinghui Li,Bolun Wang,Wentao Rao,Yanyue Wang,Hao Du,Dong Wang,Jiaqi Zhang,Xi Lin,Jianxin Zou
The magnesium-silicon hydrogen storage system (Mg 2 Si+H 2 ↔MgH 2 +Si) has attracted considerable attention with the potential of achieving near-room temperature hydrogen sorption since the reaction enthalpy is only ∼36.8 kJ/mol H 2 , offering much better thermodynamic properties over MgH 2 . However, the rehydrogenation of Mg 2 Si faces significant kinetic barriers, restricting its practical utilization. In this work, hydrogen-assisted high-energy ball milling (HHBM) was employed to hydrogenate Mg 2 Si. XRD and HRTEM results confirmed that Mg 2 Si was successfully converted into MgH 2 under the influence of titanium (Ti), achieving a conversion rate up to 76%. Aberration-corrected TEM (AC-TEM) revealed that in situ formed MgH 2 and titanium silicide (TiSi 2 ) were homogenously mixed with robust interfaces. Such a growth mode reduces the migration path of Si atoms and the stability of Mg 2 Si, thus promoting the formation of MgH 2 . Furthermore, the as-synthesized MgH 2 particles with ultrafine particle size and adjacent catalysts show superior thermolysis and hydrolysis performances. Consequently, the composite exhibits excellent hydrogen storage properties, absorbing 50% of its total hydrogen capacity at room temperature and initiating dehydrogenation at 114.3 °C. In situ synchrotron X-ray diffraction (ISXRD) confirms the dehydrogenation of in situ generated ultrafine MgH 2 and part of TiSi 2 is converted to Mg 2 Si at 283 °C. In addition, the ultrafine, defect-rich MgH 2 particles show favorable hydrolysis kinetics and high conversion efficiency at relatively low temperatures (91.9% of the hydrogen yield can be achieved at 5 °C). This method developed in this work exhibits a new way to synthesize high-performance hydrogen storage materials.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2025
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IF 8.3
Wenqiang Tang,Haoliang Tao,Yue Wang,Dianxin Wu,Bofang Zhou,Hongxia Zhang,Zhidong Chen,Chongxi Bao,Wanbin Guan,Liangzhu Zhu
Metal-supported solid oxide fuel cells (M-SOFC) possess advantages such as high mechanical strength, high toughness, good thermal conductivity, and low cost compared to traditional ceramic-supported solid oxide fuel cells, making them widely studied as a new generation of clean energy devices. When fueled with liquid ammonia, which has been recognized as a clean hydrogen carrier with a much higher volumetric energy density than compressed hydrogen, the applications of M-SOFC can be further extended such as providing continuous power source for range-extended electric vehicle. Among reported metal supports, 430L stainless steel has been considered as one of the most affordable and promising materials for M-SOFC. However, we find that when porous 430L substrate is directly exposed to non-cracked ammonia fuel, much severer corrosion and damage than dense substrate are observed, particularly at 600 °C which coincidentally fits well with desired M-SOFC working temperature imposing significant challenges for the application of 430L or other stainless steels containing Cr and Fe as supports for M-SOFC. It is found that Fe, Cr, and Ni behave quite differently at tested temperatures, and porous 430L samples show fracture as soon as after being exposed to ammonia gas at 500 °C for 10 h and at 600 °C for 1 h. Our results thus suggest that cracking of ammonia either in-situ or externally is necessary for the use of 430L substrate in M-SOFC applications.
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ChemistrySelect
·
2025
·Vol. 10
·期 13
·e202500936
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IF 2
Xiangkang Han,Juan Xia,Lingfeng Gao,Shichen Wang,Haoqi Zhan,Zhibin Han,Zeyu Wang,Xu Sun,Qin Wei
Graphical The NiFeB hydroxide (NiFeB(OH)) with nanosheet structure is fabricated via the hydrothermal reaction. Benefitted from the incorporation of electron-deficient boron (B), the formation of high-valence nickel active centers is promoted, facilitating the electrocatalytic oxidation of benzylamine. The oxidation product is benzonitrile with no by-products generated, with the Faraday efficiency being 94.15%. Considering the slow kinetics of oxygen evolution reaction (OER) and the need for high potential, organic electro oxidation, which is more prone to occur at low potential, is adopted to replace OER process. The research method combined with hydrogen evolution reaction (HER) has gradually become the mainstream direction for the synergistic production of hydrogen and high value-added organic products. In this work, the NiFeB hydroxide (NiFeB(OH)) nanosheet was prepared. Benefited from the incorporation of electron-deficient boron (B), the NiFeB(OH) catalyst exhibited excellent catalytic activity for the electrooxidation of benzylamine (BA), with benzonitrile (BN) being successfully fabricated. The experiment further proves that the conversion from BA to BN not only has high selectivity (100%) and Faraday efficiency (94.15%), but also excellent stability, which can achieve long-term operation. The excellent catalyst studied in this work provides new ideas and methods for the efficient production of benzonitrile, an organic intermediate.
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Catalysts
·
2025
·Vol. 15
·期 6
·530
·
IF 4
Yalin Guo,Zhuang Ma,Binbin Jin,Limin Ma,Guodong Yao
The sustainable valorization of lignocellulosic biomass into high-value platform chemicals presents a crucial pathway for reducing reliance on fossil resources. Gamma (γ)-valerolactone (GVL) has gained recognition as a versatile bio-derived compound with broad applications in renewable energy systems and green chemical synthesis. While conventional GVL production strategies from carbohydrate biomass typically depend on noble metal catalysts paired with high-pressure hydrogen gas, these approaches face substantial technical barriers including catalyst costs, hydrogen storage requirements, and operational safety concerns in large-scale applications. This work develops an innovative catalytic system utilizing earth-abundant iron for in situ hydrogen generation through water splitting, integrated with Raney Ni as the hydrogenation catalyst. The designed two-stage process enables direct conversion of cellulose—first through acid hydrolysis to levulinic acid (LA) followed by catalytic hydrogenation to GVL without intermediate purification. Through systematic parameter optimization, a remarkable 61.9% overall GVL yield from cellulose feedstock was achieved. Furthermore, the methodology’s versatility was demonstrated through wheat straw conversion experiments, yielding 24.6% GVL. This integrated methodology explores a technically feasible pathway for direct cellulose-to-GVL conversion utilizing abundant water as the hydrogen source, effectively overcoming the critical limitations associated with conventional hydrogenation technologies regarding hydrogen infrastructure and process safety.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Ruijie Liu,Xinhao Jiang,Xinqiang Wang,Zhenglong Li,Xiaoying Yang,Jingbo Chen,Yanxia Liu,Wengang Cui,Fan Gao,Yong Gao,Fulai Qi,Chao Zheng,Mingchang Zhang,Yaxiong Yang,Jian Miao,Lixian Sun,Jian Chen
Although Mg alloy-based hydrides have been considered as promising solid-state materials due to their high capacity and low cost, the high dehydrogenation temperature of ∼ 300℃ severely limited their practical application. Herein, a series of Mg-based quaternary alloys of Mg 85 Ni 5 Cu 5 M 5 (M = Al, Zn, Co, La) hydrides were prepared by a combination of meltspinning and ball milling process, demonstrating an efficient approach to promoting the hydrogen storage properties. Among them, the Mg 85 Ni 5 Cu 5 La 5 hydride (H-Mg 85 Ni 5 Cu 5 La 5 ) as the most excellent one starts to release hydrogen from 175℃, 125℃ lower than that of MgH 2 . Especially, the peak hydrogen release temperature of H-Mg 85 Ni 5 Cu 5 La 5 was remarkedly reduced from 347℃ to 253℃, compared with MgH 2 . Additionally, the H-Mg 85 Ni 5 Cu 5 La 5 presented an impressive initial hydrogen capacity of 4.2 wt% with a high-capacity retention of 92.6 % over 10 dehydrogenation cycles. In/Ex-situ XRD analyses proved that the synergistic effects of in-situ formed metallic Ni and LaH 2 catalytic phases during the milling and ab/desorption processes can simultaneously enhance the ab/desorption kinetics of Mg/MgH 2 . That is, the LaH 2 can act as a hydrogen pump to promote the dehydrogenation of hydrides, while the Ni is beneficial to accelerate the dissociation of metal-hydrogen atoms and the formation of hydrogen molecules on the surface of Mg alloy. These findings highlight the potential of multicomponent Mg-based alloys for practical use in solid-state hydrogen storage systems through in-situ formed catalytic phases.
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ACS Applied Energy Materials
·
2025
·
IF 5.5
Mingxing Guo,Aojie Zhang,Chao Wu,Wenhao Fan,Qiang Zhang,Shaoping Chen
The n-type Mg3(Sb,Bi)2-based thermoelectric materials are promising candidates for medium-temperature power generation due to their low cost, nontoxicity, and high performance. However, their large-scale application in thermoelectric devices is significantly hindered by poor long-term stability, resulting from electrode interface degradation. Effective contact interfaces in thermoelectric devices require high bonding strength, low interfacial resistivity, and exceptional stability. Therefore, the development of efficient and reliable thermoelectric interface materials is crucial for the practical application of these devices. Conventional approaches to forming interfacial barrier layers mainly rely on thermodynamic equilibrium, which often overlook the critical roles of interfacial reactions and diffusion kinetics. In this study, molecular dynamics simulations were employed to uncover the underlying mechanisms responsible for the high stability of the Mg2Ni barrier layer and its interface with thermoelectric materials. The Mg2Ni/Mg3.21Sb1.5Bi0.5Y0.04 thermoelectric device exhibited excellent performance, with a low contact resistance of 11 μΩ·cm2, a high output power density of 1.2 W·cm–2, and an energy conversion efficiency of 5% at a temperature difference of ΔT = 373 K. This strategy is applicable to other thermoelectric materials, offering valuable insights for designing barrier layers in diverse thermoelectric systems.
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