ACS Sustainable Chemistry & Engineering
·
2026
·
IF 7.6
Jiang Tian,Chen Junjie,Lei Ying,Tao Zhilin,Li Jiaxin,Han Wenjing,Cheng Zheng,Zhang Bin,Li Jianying
Ni-rich layered oxide cathodes received considerable research interest due to their high energy density, yet their cycling stability was severely limited by irreversible H2–H3 phase transition-induced lattice strain accumulation and lattice oxygen release, especially at high voltage. Here, we report a coherent twin-phase engineering strategy by doping trace antimony (Sb) to stabilize layered LiNi 0.82 Co 0.12 Mn 0.06 O 2 (NCM) cathodes under deep delithiation. Aberration-corrected STEM reveals Sb-induced coherent twin phases that crystallographically connect layered and locally rocksalt-like domains while maintaining an intact layered oxygen framework. These coherent twin phases act as robust pinning interfaces that suppress irreversible H2–H3–induced c -axis contraction and mitigate anisotropic lattice stress during high-voltage cycling. Meanwhile, time-of-flight secondary ion mass spectrometry and theoretical calculations reveal that strengthened Sb–O bonding raises the oxygen-vacancy formation energy, stabilizing lattice oxygen and suppressing oxygen release, thereby preserving structural integrity and mitigating transition-metal dissolution. Benefiting from these synergistic stabilization effects, 0.75Sb-NCM exhibits a high discharge capacity of 209.61 mAh g –1 at 0.1 C and maintains 85.56% capacity retention after 200 cycles at 1 C within 2.8–4.5 V, significantly outperforming U-NCM (70.22%). This work highlights coherent twin phases as a robust structural pinning architecture for stabilizing Ni-rich layered cathodes at high states of charge.
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ACS Applied Materials & Interfaces
·
2026
·Vol. 18
·期 30
·40660-40671
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IF 7.8
Jin Zhao,Yao Shunyu,Sun Chang,Zhang Chunqi,Liang Licheng,Liu Yipeng,Yang Qingqing,Liang Fei
The practical deployment of magnesium-based alloys, despite their attractive hydrogen-storage capacity and economical advantage, faces critical barriers in the form of high dehydrogenation temperatures and inadequate sorption kinetics. To overcome these barriers, a two-dimensional layered La x @Ti 3 C 2 -derived catalyst was therefore developed, which exhibits high catalytic activity toward the Mg-4Ni-2Y alloy. The Mg-4Ni-2Y + 10 wt % La 0.2 @Ti 3 C 2 composite not only lowered the onset absorption/desorption temperatures to 23.3 ° C and 265.5 ° C but also enabled the composite to achieve superior sorption kinetics, absorbing 4.80 wt % H 2 in 1 min at 150 ° C and releasing 5.16 wt % H 2 in 4 min at 350 ° C. Furthermore, the apparent activation energy (E a ) was substantially reduced to 85.22 ± 2.38 kJ/mol for the composite, thereby decreasing the dehydrogenation temperature and accelerating the kinetics. Systematic analysis suggests that the catalytic enhancement is primarily associated with highly dispersed Ti 0 species, which are proposed to act as the primary active sites for hydrogen dissociation and recombination. La decoration is suggested to serve as an electronic promoter, modulating the electronic structure of Ti sites and stabilizing the interfacial environment. This synergistic Ti-La interaction facilitates hydrogen activation and interfacial transfer without altering the intrinsic Mg/MgH 2 thermodynamics, thereby significantly accelerating hydrogen sorption kinetics.
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ACS Applied Materials & Interfaces
·
2026
·
IF 7.8
Cai Qingmei,Su Shengqi,Zhang Yunsheng,Yang Wenxiu,Zhang Wenhui,Lin Xijie
Ni-rich layered oxides, benefiting from their superior specific capacity, have emerged as pivotal cathode candidates for high-energy-density lithium-ion batteries (LIBs). Nevertheless, these materials suffer from severe intrinsic interfacial and structural degradation under high-voltage operation, which severely compromises their practical electrochemical performance. Herein, we developed a surface-bulk phase differentiated modification strategy integrating CeO 2 coating and Fe 3+ doping, leveraging the divergent diffusion behaviors induced by the different ionic radii of Ce 3+ and Fe 3+ ions. This targeted modification approach effectively mitigated the interfacial degradation and bulk structural deterioration of Ni-rich cathode materials. Specifically, the surface CeO 2 coating inhibited parasitic reactions at the cathode–electrolyte interface, and its rich oxygen vacancies efficiently suppressed lattice oxygen release during long-term cycling. Meanwhile, bulk Fe 3+ doping reduced Li + /Ni 2+ cation mixing, alleviated internal lattice strain, and reinforced the crystal framework. The synergistic effect of CeO 2 coating and Fe 3+ doping endowed the cathode with optimized interfacial integrity and structural durability. Taking LiNi 0.83 Co 0.11 Al 0.06 O 2 as a representative material, the CeO 2 -coated and Fe 3+ -doped cathode demonstrated significantly improved cycling performance at conventional 4.3 V and elevated 4.5/4.6 V. Specifically, after 200 cycles at 1 C within 3.0–4.6 V, the modified cathode retained a capacity retention of 76.9%, which was much higher than the 61.7% retention of the pristine sample. This study highlights the great potential of surface-bulk phase differentiated engineering for stabilizing Ni-rich cathodes, providing a feasible pathway for the development of high-energy-density LIBs.
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LANGMUIR
·
2026
·
IF 4.4
Jing Zhang,Shiyao Hou,Xindi He,Haiming Li,Xing Wang,Ziqing Gao,Yanzhu Guo
Green fluorescent protein (GFP) is widely utilized as a fluorescent probe in biomedical research, yet its high-purity separation remains challenging. Traditional purification methods often involve complex procedures, high costs, and environmental concerns. In this study, a dual-functional bacterial cellulose-based hydrogel (BPP) was successfully fabricated via graft copolymerization of acrylic acid (AA) and acrylamide (AM) onto the BC framework. The resulting hydrogel exhibited a highly hydrated three-dimensional network with outstanding mechanical properties and swelling rate (compressive strength: 1.54 MPa; 300 compression cycles at 80% strain: 90% stress retention). The maximum adsorption capacity of BPP for Ni(II) was 315.9 mg/g (T = 55 °C) and effectively suppressed metal ion leaching while generating abundant coordination-active sites for selective GFP capture (228.9 mg/g). Notably, the captured GFP retained high fluorescence activity and could be efficiently eluted using imidazole buffer, with a recovery rate of 61.1%. Spectroscopic analyses (FT-IR and XPS) revealed a sequential adsorption mechanism involving strong chelation of Ni(II) by polymeric carboxyl and amino groups, followed by Ni(II)-mediated specific coordination with His-tagged GFP. This work demonstrates a sustainable polymer-based strategy that integrates heavy metal ion immobilization with high-value protein purification, highlighting the potential of multifunctional cellulose hydrogels for advanced bioseparation and the design of resource-oriented materials.
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RENEWABLE ENERGY
·
2026
·
IF 9.1
Quanxiong Lu,Xianliang Song
Direct lignin fuel cells (DLFC) have recently attracted much attention. However, there are few reports on preparing anodic catalytic layer for DLFC. Thereby, we loaded a small amount of platinum carbon (Pt/C) catalyst on the surface of nickel (Ni) foam by a simple roller pressing method, thus realizing the preparation of Pt-Ni/C bimetallic catalysts. The results proved the successful loading of the Pt/C catalyst onto nickel foam, and the catalyst particle size has an average size of 2.76 nm. The Pt-Ni/C catalysts not only have good oxygen evolution reaction (OER) activity (154 mV overpotential@10 mA/cm 2 and tafel-slope of 44 mV/dec) but also have good lignin oxidation reaction (LOR) activity with a low overpotential of 247 mV at 10 mA/cm 2 . Pt-Ni/C catalysts were applied to DLFC at room temperature, showing an open-circuit voltage (OCV) of 0.84 V and a maximum power density of 0.62 mW/cm 2 . The optimum Pt/C loading was found to be 0.5 mg/cm 2 . The modified DLFC is comparable to glucose fuel cells' power generation performance and shows better application prospects.
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ACS Sustainable Chemistry & Engineering
·
2026
·
IF 7.6
Qiaozhi Han,Chengxu Li,Yunshu Wang,Ziwei Ma,Chengyu Duan,Yucong Yin,Zichen Bao,Yonghao Shen,Chenwen Yin,Zhuofeng Hu,Qiming Sun
Abstract The direct synthesis of hydrogen peroxide (H2O2) from H2 and O2 provides a sustainable route for decentralized oxidant production, but its practical use is limited by inefficient Pd utilization, undesired H2O2 decomposition, and the need for high noble-metal loadings. Here, we report a Ni(OH)2-promoted Pd@S-1 catalyst that integrates zeolite confinement with interfacial electronic modulation for efficient aqueous H2O2 synthesis. The optimized Pd4Ni1@S-1-H catalyst delivers an H2O2 productivity of 3.39 mol gPd–1 h–1 under acidic conditions, representing the highest value among reported semibatch glass reactor systems and a 10-fold improvement in Pd utilization efficiency relative to a commercial Pd/C catalyst. Advanced spectroscopic analysis and density functional theory calculations reveal that Ni(OH)2 donates electrons to Pd, lowering the average Pd valence state from 1.83 to 1.39, and serves as a hydrogen-transfer bridge that promotes hydrogen migration to the *O–O intermediate. Meanwhile, hydrophobic silicalite-1 (S-1) zeolite micropores enrich dissolved H2/O2 and suppress secondary H2O2 decomposition by facilitating product desorption. The resulting in situ H2O2 generation system enables efficient Cr(VI) reduction, highlighting its potential for sustainable water remediation.
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MICROCHEMICAL JOURNAL
·
2026
·
IF 5.2
Lei Jiang,Chunli Mao,Gaojie Cheng,Hongbo Yang,Jiawen Yin,Qinghui Jin
An integrated three-electrode non-enzymatic urea sensor is developed. • The sensor exhibits a wide linear range (1–200 mg/L) and a fast response (10.8 s). • Detection potential dynamically regulates the contributions of the two urea oxidation pathways. Rapid and accurate monitoring of urea concentration in swimming pool water is critical for protecting swimmers' health and optimizing water quality management. However, traditional techniques are either expensive or operationally complex, whereas enzyme-based sensors suffer from enzyme deactivation, limiting their applicability for online monitoring. In this paper, a nickel hydroxide/nickel oxyhydroxide (Ni(OH) 2 /NiOOH) nanonetwork electrochemical sensor for non-enzymatic urea detection is proposed, which is mass-produced on a platinum electrode using microelectromechanical systems (MEMS). The electrode was activated and optimized via cyclic voltammetry by varying the scan rate. The sensor demonstrates a high sensitivity of 1.43 μA/(mg·L −1 ·cm 2 ), a wide detection range of 1–200 mg/L, a fast response time (<12 s), good repeatability with a relative standard deviation (RSD) of 1.24%, and an excellent linearity ( R 2 = 0.9988). In addition, the proposed sensor exhibits excellent anti-interference performance toward coexisting species such as creatinine, uric acid, residual chlorine, and lactic acid. Practical applications in swimming pool water samples yielded recovery rates of 92.5–100.4%, validating the sensor's robustness. Two distinct oxidation mechanisms for urea on the electrode were observed by electrochemical impedance spectroscopy (EIS). The direct pathway was further found to be potential-tunable, with its charge-transfer resistance decreasing by 35.6% upon raising the working potential from 0.45 V to 0.50 V. This work offers a promising route toward non-enzymatic urea sensors for swimming pool water monitoring. Download: Download high-res image (140KB) Download: Download full-size image
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Science Advances
·
2025
·Vol. 11
·期 24
·
IF 12.5
Jian-Yu Zou,Fang-Li Xing,Quan-Xing Zi,Hai-Wu Du,Meiwan Chen,Wei Shu
α-Chiral phosphorus compounds have broad applications as organic catalysts or ligands in organic chemistry and related areas. Herein, we disclose a Ni-catalyzed enantioselective cross-hydrodimerization of alkenyl phosphine sulfides with unactivated alkenes to access α-chiral phosphine sulfides, representing the first example of asymmetric hydrodimerization of electron-deficient alkenes with electron-rich alkenes. Key to success is the precise recognition between electron-deficient alkenes and electron-rich alkenes and streamlined alkyl-alkyl bond forming with the control of chemo-, regio-, and enantioselectivity. This strategy requires alkenes as sole precursors for asymmetric alkyl-alkyl cross-coupling, circumventing the use of stoichiometric amounts of alkyl electrophiles or alkyl nucleophiles as coupling partners. The mild conditions tolerate a wide range of functional groups, providing direct access to α-chiral phosphines through a carbon-carbon bond-forming process without prefunctionalized coupling precursors.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Tengyu Zhang,Meijia Liu,Fangyi Wu,Yuanhang Wang,Yujia Ma,Lu Wang,Fangong Kong
Magnesium hydride (MgH 2 ) is regarded as a promising solid-state hydrogen storage material with high capacity and abundant resources, while its large-scale application is limited because of the inherent thermodynamic and kinetic issues. In this study, a nitrogen-doped carbon-coated Ni/MnO nanosphere catalyst (Ni/MnO@NC) was synthesized to enhance the hydrogen storage performance of MgH 2 by lowering the operating temperature and improving kinetic properties. Incorporation of 10 wt% Ni/MnO@NC lowered the onset dehydrogenation temperature of MgH 2 to 225.2 ℃ and reduced the dehydrogenation activation energy to 97.68 kJ/mol. At temperatures as low as 50 ℃, MgH 2 -Ni/MnO@NC composite achieved 2.92 wt% hydrogen absorption within 30 min. Moreover, the composite retains 97.4 % of its initial capacity after 30 cycles. Mechanistic analysis indicates that the superior hydrogen storage performance arises from synergistic catalysis among intermediate and derived phases, including the hydrogen pump effect of Mg 2 Ni/Mg 2 NiH 4 , enhancement of electron transfer by multivalent Mn, and suppression of MgH 2 particle aggregation and growth by nitrogen-doped carbon. These findings put forward a promising strategy to advance the practical application of MgH 2 in hydrogen storage systems.
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CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
·
2025
·
IF 3
Zhang Wen,Zhang Ning,Gao Jianyang,Liu Fusheng,Zhang Yang,Xu Guang-Rui,Wang Lei
Recently, zinc-air batteries have been of great interest due to their high theoretical specific energy that plays an important role in renewable energy conversion, while the sluggish kinetics of their half-reactions of oxygen reduction and oxygen evolution (ORR/OER) limit their widespread applications. Herein, we report the synthesis of self-assembly Ni@PdNiO x seashell-like nanostructures (Ni@PdNiO x NSs) with low Pd content through a novel one-step wet chemical method for the first time. The optimized self-assembly Ni@PdNiO x NSs with a thickness of 2.06 nm are connected self-assembled to form a network structure, which exhibits a large surface area and unprecedented ORR/OER with a positive half-wave potential of 0.892 V vs. RHE and an overpotential of 230 mV at 10 mA/cm 2 in alkaline solution, outperforming most of the PdNi catalysts. When the self-assembly Ni@PdNiO x NSs are applied as electrodes for zinc-air batteries, they deliver a high power density of 88.9 mW/cm 2 and an impressive energy density of 714 mA·h·g −1 . This work opens up a new strategy for generating superior oxygen electrocatalysis and provides new insight into the correlation of low Pd content and Ni in the improvement of alkaline oxygen electrocatalysis.
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IONICS
·
2025
·
IF 2.6
Liu Dongni,Guo Lichi,Duan Ruochen,Zhang Shengwei,Li Mingying
Microbial fuel cells (MFCs) represent an emerging energy technology that generates electricity through microbial-organic interactions, with the anode serving as a critical component for wastewater-to-electron conversion. This study focuses on developing porous iron-nickel (Fe–Ni) alloys as potential anodes for MFCs, employing electrodeposition to fabricate these anodes with systematically varied Fe/Ni ratios. Through intrinsic electrochemical performance screening, the work aims to achieve composition optimization for high-performance microbial fuel cell anodes. Multi-dimensional analysis integrating linear sweep voltammetry (LSV), cyclic voltammetry (CV), electrochemical impedance spectroscopy (EIS), and Tafel polarization was conducted to establish structure–activity relationships and synergistic catalytic mechanisms of the alloys. Key findings reveal that compositional optimization profoundly impacts the performance of these potential anodes: the Fe 7 Ni 3 alloy exhibited significantly superior electrochemical activity compared to pure Ni, characterized by dramatically enhanced peak current density, and improved charge storage capacity. Furthermore, Fe 7 Ni 3 demonstrated minimal charge transfer resistance and excellent reaction kinetics. These results validate that bulk composition engineering of porous Fe 7 Ni 3 offers a highly promising strategy for developing potential anode materials for high-performance MFCs, effectively addressing the stability-activity trade-off inherent in conventional surface-modified anodes. This work provides a composition-driven design paradigm for bioelectrochemical systems, paving the way for future scale-up studies focusing on long-term stability and integration into wastewater treatment modules. Graphical abstract
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ACS Applied Nano Materials
·
2025
·
IF 5.5
Jiaxin Li,Junhui Liang,Xin Yao,Hongming Liu,Yuhui Du,Huayu Chen,Hangning Chen,Chenhao Du,Liuqi Wang,Yincheng Li,Yuexiang Huang,Da Chen
The development of low-temperature, nonprecious metal thermocatalysts for ammonia decomposition holds significant promise for advancing the green hydrogen industry. LaNiO3 catalysts, with their perovskite structure (ABX3), are notable for enabling in situ growth of active metal Ni on reduced oxide supports during ammonia decomposition reactions (ADRs). However, unintentional in situ growth can lead to uncontrolled reactions and metal particle agglomeration. To address this, we employed a straightforward high-temperature and pressure hydrogenation pretreatment process to enhance the interaction between the active metal and the support, thereby suppressing the agglomeration of the active metal during the ADR process. Our results indicate that the hydrogenation pretreatment catalyst exhibits finer Ni metal nanoparticles, with an average size of approximately 8 nm. Under a gas hourly space velocity (GHSV) of 18,000 mL gcat–1 h–1 and at 550 °C, the NH3 conversion efficiency reaches 90%, which exhibited excellent stability over a period of 100 h. Additionally, we utilized TEM, XPS, EPR, NH3-TPD, and H2-TPR techniques to elucidate the intrinsic mechanisms related to the enhanced catalytic activity. This study addresses the issue of active metal nanoparticle agglomeration through hydrogenation pretreatment.
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