ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Yuting He,Junbo Yang,Yi Wang,Yufei Jia,Hongtao Li,Yongning Liu,Liting Liu,Qiang Tan
The metal–nitrogen–carbon (M–N–C)-based catalysts are promising to replace PGM (platinum group metal) to accelerate oxygen reduction reaction due to their excellent electrocatalytic performance. However, the inferior intrinsic activity and poor active site density confining further improvement in their performance. Modulating the electronic structure and reasonably designing the pore structure are widely acknowledged effective strategies to boost the activity of the M–N–C catalysts. However, it is a great challenge to form abundant pores to regulate the electronic structure via the facile method. Herein, a hierarchical, porous dual-atom catalyst FeNi-NPC-1000 has been architectured by the Na2CO3 template method and bimetallic doping modification strategy. Benefitting from the optimized pore and electronic structure, the as-prepared FeNi-NPC-1000 possesses a high specific surface area (1412.8 m2 g–1) and improved ORR activity (E1/2 = 0.877 V vs RHE), which is superior to that of Pt/C (E1/2 = 0.867 V vs RHE). With the evidence of AC-STEM, XAS, and DFT, the FeNi-N8-C moiety is proven to be the key active site to realize high-efficiency ORR catalysis. When assembled it as an air cathode of ZABs, FeNi-NPC-1000 displays superior discharge performance (Pmax = 367.1 mW cm–2) and a stable battery long-life. This article will provide a new strategy for designing dual-metal atomic catalysts applied in metal–air batteries.
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AICHE JOURNAL
·
2025
·
IF 4
Hui Wang,Yifan Jin,Yaxin Jin,Siyu Kuang,Tianxiang Yan,Xinyue Wang,Xiao Wang,Wenquan Cui,Sheng Zhang
Electrochemical carbon dioxide reduction reaction (CO 2 RR) is one of the most prospective strategies to achieve carbon neutrality. Multi-carbon compound (C 2+ ) products have higher commercial value and wider applications, among which ethanol is a widely used chemical feedstock and high energy density fuel. Here, we prepared nitrogen-doped carbon nanofibers containing copper-zinc double atoms using the electrospinning technique and controlled the content of both metal atoms by varying the calcination temperature. This catalyst exhibited ultra-high selectivity for ethanol at low potentials. Ethanol selectivity at −0.3 V versus RHE was more than 60% with the total alcohol selectivity of over 80%. Meanwhile, we explored the ethanol production pathway by combining density-functional theory (DFT) and ATR-FTIR spectroscopy, and found that OCCO* intermediates were most abundant for the optimal ratio of Cu to Zn atoms, lowering the energetic barriers to ethanol formation, and thus improving the selectivity of ethanol production.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Xinliang Han,Xiangyu Kong,Dewei Wang,Xu Li,Liubing Dong
Zn-ion hybrid capacitors (ZICs) are a novel and promising electrochemical energy storage system, while exploring high-performance cathode materials is essential for the development of ZICs. Herein, we propose hydrous ruthenium oxide quantum dots (RuO 2 QDs) anchored on porous carbon nanocages (PCNCs) as a new cathode material for ZICs. For the RuO 2 QDs@PCNCs material, hydrous RuO 2 QDs with a small size of 2–3 nm uniformly disperse on the PCNC support, providing large electrode–electrolyte interface for electrochemical reactions and abundant active sites for ion storage. Consequently, the RuO 2 QDs@PCNCs cathode material displays desirable electrochemical performance in ZICs, including a large capacity of 224 mAh g −1 at 0.4–1.8 V, superior rate capability (showing 156 mAh g −1 capacity even at a large current of 20 A g −1 ) and good stability during a long-term cycling test over 20,000 cycles, significantly superior to currently-reported cathode materials for ZICs. An ultrahigh energy density of 180 Wh/kg is achieved for the RuO 2 QDs@PCNCs cathode-based ZICs. Mechanism investigations point out the capacitive behavior-dominated and Zn 2+ /H + co-participated charge storage process with fast electrochemical kinetics for the RuO 2 QDs@PCNCs cathode in ZICs. This work not only provides a new choice for high-performance cathodes but also enriches the electrochemical theory of ZICs.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yiyi Zhang,Minfeng Chen,Junjie Lu,Hong Ma,Wenhui Liu,Jingxuan Yu,Qinghua Tian,Junling Xu,Jizhang Chen
Aqueous zinc-ion batteries hold substantial promise, benefiting from their cost-effectiveness, high safety, and impressive power density. Nonetheless, their performance is compromised by Zn dendrites and by-product formation at the Zn anode. Hydrogel electrolytes are considered a viable solution to these issues. This study proposes to fabricate anisotropic carboxymethyl cellulose hydrogel electrolyte with aligned channels through a straightforward directional freezing technique, aiming to simultaneously achieve good mechanical properties and large ionic conductivity. Meanwhile, Zn(ClO 4 ) 2 is introduced into hydrogel electrolyte to establish ternary hydrogen-bonding network, so as to enhance frost resistance. Thanks to these benefits, the anisotropic hydrogel electrolyte (denoted as Ani-hydrogel) manifests improved Zn 2+ ion transfer, expedited desolvation process, favored planar Zn 2+ ion diffusion, and promoted interfacial kinetics. Accordingly, Zn dendritic growth and parasitic reactions can be efficiently impeded, contributing to significantly improved reversibility of Zn stripping/plating. With the use of Ani-hydrogel electrolyte, the duration of Zn//Zn cell is extended to 1200 h under 2 mA cm −2 and 2 mAh cm −2 , and the Zn//Cu cell can be stably operated for 300 cycles. The Zn//MnO 2 battery with Ani-hydrogel electrolyte delivers superior cyclability at both room temperature and –10 ℃. This study underlines the importance of anisotropic architecture for hydrogel electrolytes.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2025
·
IF 7.7
Lin Li,Daocheng Hong,Bohao Liu,Tianci Su,XiuLi Yang,Lu Yue,Wenhui Zhang
Porous zinc doped indium oxide (Zn-In 2 O 3 ) nanobelts were synthesized using a straightforward hydrothermal method. The effects of different metal doping (Zn, Sn, Sm, Yb, Cu) and various concentrations of Zn on the morphology and gas-sensing properties of In 2 O 3 were investigated. The gas sensing evaluations reveal that among all tested sensors, the porous 7.5% Zn-In 2 O 3 nanobelt sensor exhibits the highest response, reaching 127 (S= R a / R g ) to 50 ppm acetone at a low operating temperature of 140°C, which is approximately 21 times greater than that of pure In 2 O 3 . Additionally, this sensor demonstrates rapid response/recovery time, a low detection limit of 40 ppb, good selectivity, excellent repeatability, and long-term stability toward acetone. In-situ diffuse reflectance infrared Fourier transform (DRIFT) spectroscopy and density functional theory (DFT) calculations are employed to elucidate the mechanisms behind the enhanced gas-sensing performance of the porous Zn-In 2 O 3 nanobelts. The superior gas-sensing characteristics are attributed to the distinctive porous nanobelt architecture, abundant oxygen vacancies, large specific surface area, and the effects of Zn doping.
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DALTON TRANSACTIONS
·
2024
·Vol. 53
·期 6
·2526-2533
·
IF 3.5
Jia-Min Lyu,Shen Yu,Zhan Liu,He-You Du,Ming-Hui Sun,Chun-Mu Guo,Yi-Long Wang,Yu Li,Li-Hua Chen,Bao-Lian Su
Excessive emission of CO2 into the atmosphere has severely impacted the global ecological environment. Converting CO2 into valuable chemicals and fuels is of great significance for sustainable development. However, low activity and undesirable selectivity often result from the inherent inertness of CO2. Herein, K- or/and Zn-modified Fe-based catalysts were prepared by an incipient-wetness impregnation method for CO2 hydrogenation via a cascade reaction. The results indicate that K species exist as K2O while Zn species exist as ZnFe2O4. In the CO2 hydrogenation pathway, K2O facilitates the adsorption of CO2 and restrains the adsorption of H2, accelerating the transformation of CO2 into C2–C4 olefins rather than paraffins while Zn species promote the dispersion of Fe species, leading to improved activity. Synergistically, a K- and Zn-modified Fe-based catalyst (2Zn–10K–Fe/Al) shows excellent catalytic CO2 hydrogenation activity, achieving a CO2 conversion of 77% which is 1.8 times that (42%) of the unmodified Fe-based catalyst (Fe/Al). Our catalyst also shows a significantly promoted selectivity to C2–C4 olefins of 17% in comparison with the Fe/Al catalyst (0%). It is envisioned that such a binary effect of elements might contribute to the low-cost and industrial production of Fe-based catalysts for selective CO2 conversion.
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LANGMUIR
·
2024
·
IF 3.7
Xue Chen,Yong Xiang,Xiaojing Zhang,Guanlin Li,Sihan Ai,Daoyong Yu,Baosheng Ge
Carbonic anhydrase (CA) plays a crucial role in the CO2 capture processes by catalyzing the hydration of CO2. In this study, we synthesized a bioinspired carbonic anhydrase Zn-MOF (metal–organic framework) incorporating 2-aminoimidazole and Zn2+ as initial constituents. The synthesized Zn-MOF exhibited promising potential for efficiently catalyzing the CO2 hydration. Structural analyses such as SEM, XRD, and BET confirmed that the Zn-MOF crystal consisted of stacked grains with an average size of approximately 36 nm, forming a micron-sized spherical structure. Functionally, Zn-MOF exhibited effective catalytic activity toward both CO2 hydration and ester hydrolysis. The introduction of amino groups significantly enhanced the esterase activity of Zn-MOF to 0.28 U/mg at ambient temperature, which was twice that of ZIF-8. Furthermore, the introduction of amino groups resulted in remarkable hydrothermal stability, with the esterase activity reaching 0.72 U/mg after undergoing hydrothermal treatment at 80 °C for 12 h. Additionally, Zn-MOF exhibited enhanced capability in CO2 hydration at a pH value exceeding 8.5. After six repeated uses, ZIF-8 and Zn-MOF retained approximately 68 and 65% of their initial enzyme activity, respectively, underscoring the potential practical applicability of Zn-MOF in industrial CO2 capture processes. This work showcases the development of a novel Zn-MOF crystal as an efficient CA mimic, effectively emulating the active sites of natural CA using 2-aminoimidazole as a coordinating ligand for Zn2+ coordination. These findings not only advance the field of innovative enzyme mimics but also pave the way for further exploration of industrial CO2 capture catalysts.
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MOLECULES
·
2024
·Vol. 29
·期 14
·3416
·
IF 4.2
Binrui Xu,Yong Liu,Bo Zhao,Haoming Li,Min Liu,Huanxiao Mai,Quanan Li
Electrolyte additive engineering is a crucial method for enhancing the performance of aqueous zinc—ion batteries (AZIBs). Recently, most research predominantly focuses on the role of functional groups in regulating electrolytes, often overlooking the impact of molecule stereoscopic configuration. Herein, two isomeric sugar alcohols, mannitol and sorbitol, are employed as electrolyte additives to investigate the impact of the stereoscopic configuration of additives on the ZnSO4electrolyte. Experimental analysis and theoretical calculations reveal that the primary factor for improving Zn anode performance is the regulation of the solvation sheath by these additives. Among the isomers, mannitol exhibits stronger binding energies with Zn2+ions and water molecules due to its more suitable stereoscopic configuration. These enhanced bindings allow mannitol to coordinate with Zn2+, contributing to solvation structure formation and reducing the active H2O molecules in the bulk electrolyte, resulting in suppressed parasitic reactions and inhibited dendritic growth. As a result, the zinc electrodes in mannitol—modified electrolyte exhibit excellent cycling stability of 1600 h at 1 mA cm−2and 900 h at 10 mA cm−2, respectively. Hence, this study provides novel insights into the importance of suitable stereoscopic molecule configurations in the design of electrolyte additives for highly reversible and high—rate Zn anodes.
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ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Ze Li,Yidan Fu,Lina Han,Pengfei Zheng,Xiaoyuan Zeng,Peng Dong,Jing Feng,Yingjie Zhang
The insufficient d-electron density in V metal atoms limits O2 dissociation, constraining the kinetics and activity of the oxygen reduction reaction and the oxygen evolution reaction in VN-based catalysts. Herein, Co dopant was employed to modulate the electronic characteristics of the d-orbitals and associated free energy of VN, thereby further enhancing its catalytic activity. XPS and XANES spectra revealed that Co atoms replaced V and strongly bonded with neighboring N atoms, effectively regulating the local electronic structure. DFT analysis show that the Co doping strategy effectively regulates the adsorption/desorption equilibrium of oxygen reduction reaction intermediates through d-electron transfer to V atoms, while significantly lowering the activation energy barrier of the rate-determining step. Electrochemically, V0.95Co0.05N/NC/C achieved a low bifunctional index (ΔE = 0.78 V), with a half-wave potential for the ORR of 0.83 V and an OER overpotential of 380 mV at 10 mA cm–2. In Zn-air batteries, it achieved a high specific capacity (708.98 mAh gZn–1) and retained 88% initial voltage after 280 h cycling, demonstrating robust stability for practical applications. This study presents a doping strategy to modulate d-band centers in transition metal nitrides for energy conversion devices.
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ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Yuhan Fu,Yali Li,Yang Chen,Jidong Hu,Hai Liu,Jiawei Zhao,Shoukun Zhao,Hongyun Ma,Yujun Fu,Deyan He,Junshuai Li
The performance of aqueous zinc-ion batteries is frequently hindered by anode-related issues such as uncontrolled dendrite formation and side reactions. Metal–organic frameworks (MOFs), characterized by their highly ordered porous structures, remarkably large specific surface areas, and tunable active sites, offer a promising solution by regulating Zn2+ flux and promoting uniform Zn deposition. In this study, a Cu-MOF was synthesized in situ on carbon cloth (CM-C) and functioned as an ion-buffering layer within the battery. This innovative configuration significantly mitigates side reactions, achieving an extended cycle life of nearly 800 h at a high current density of 10.0 mA cm–2 (areal capacity: 10.0 mA h cm–2) and nearly 1200 h at 5.0 mA cm–2. After 2000 cycles at 5.0 mA cm–2, the battery demonstrated an average Coulombic efficiency of 99.3%. Additionally, the full battery containing CM-C demonstrated enhanced capacity and stability. This simple and novel structure provides new possibilities for enhancing the cycling stability of zinc-ion batteries.
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CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Yang Chen,Diwen Zhou,Yongli Chang,Hongqiao Lin,Yunzhao Xu,Yong Zhang,Ding Yuan,Lizhi Wu,Yu Tang,Chengyi Dai,Xingang Li,Qinhong Wei,Li Tan
CO 2 hydrogenation to CH 3 OH is of great significance for achieving carbon neutrality. Here, we show a urea-assisted grinding strategy for synthesizing Cu-Zn-Ce ternary catalysts (CZC-G) with optimized interfacial synergy, achieving superior performance in CO 2 hydrogenation to methanol. The CZC-G catalyst demonstrated exceptional methanol selectivity (96.8%) and a space-time yield of 73.6 g MeOH ·kg cat –1 ·h –1 under optimized conditions. Long-term stability tests confirmed no obvious deactivation over 100 h of continuous operation. Structural and mechanistic analyses revealed that the urea-assisted grinding method promotes the formation of Cu/Zn-O v -Ce ternary interfaces and inhibits the reduction of ZnO, enabling synergistic interactions for efficient CO 2 activation and selective stabilization of formate intermediates (HCOO*), which are critical for methanol synthesis. In-situ diffuse reflectance infrared Fourier transform spectra and X-ray absorption spectroscopy studies elucidated the reaction pathway dominated by the formate mechanism, while suppressing the reverse water-gas shift reaction. This work underscores the critical role of synthetic methodologies in engineering interfacial structures, offering a strategy for designing high-performance catalysts for sustainable CO 2 resource utilization.
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MATERIALS RESEARCH BULLETIN
·
2025
·
IF 5.7
You Li,Yunshu Zhang,Zhichao Gan,Lulu Zhan,Yanan Ji,Mengxue Zhou,Yi Lin
Aqueous zinc-ion batteries (AZIBs) promise safe, green and cheap grid storage.Among the cathode candidates, α-MnO₂ is regarded as one of the most promising materials yet they are throttled by poor conductivity.In this work, a microwave-hydrothermal route is adopted to rapidly tailor the crystal orientation and micro-morphology of α-MnO₂, and the correlation between microstructure and ion-diffusion kinetics is systematically investigated. Graphene (Gr) is subsequently introduced to construct a three-dimensional conductive network, which markedly lowers charge-transfer resistance. Quantitative pseudocapacitive analysis further elucidates the underlying energy-storage mechanism. It is revealed that a properly prolonged hydrothermal duration alleviates nanorod aggregation, enlarges the specific surface area, and thus accelerates ion diffusion. Concurrently, the Gr-incorporated architecture enables rapid Zn²⁺/H⁺ transport and endows the composite with superior reaction kinetics. Consequently, a synergistic enhancement in both specific capacity and cycling stability is achieved. This work offers a feasible strategy for the rational design of high-performance Mn-based cathodes.
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