ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Maosheng Gong,Yadong Wei,Hongzhou Zhang,Jingyuan Liu,Xin Zhang,Xuanming Chang,Peiyu Hou,Xijin Xu,Lianqi Zhang
High-capacity Ni-rich cathodes hold considerable promise in advancing both high-energy Li-ion batteries (LIBs) and all-solid-state Li batteries (ASSLBs). Yet, lattice volume changes induced by the H2–H3 phase transition lead to structural degradation. It has been demonstrated that doping approaches can enhance structural stability. Nevertheless, the selection of an appropriate dopant is of considerable importance for the design of high-performance Ni-rich materials with high-entropy doping. Furthermore, the feasibility of high-entropy doped Ni-rich cathodes in ASSLBs has not been reported to date. In this study, leveraging the chemically competitive doping mechanism of Mg, Al, Ti, Nb, and Mo elements, we propose a high-entropy doped LiNi0.8Co0.1Mn0.05Mg0.01Al0.01Ti0.01Nb0.01Mo0.01O2 (HE-NCM) to stabilize Ni-rich cathodes. In-situ X-ray diffraction confirms that the synergistic effect of multiple dopants in high-entropy doping significantly alleviates the H2–H3 phase transition and reduces lattice volume changes, which contribute to the absence of microcracks and improved bulk/interface stability. In ASSLBs, the HE-NCM@LiNbO3 maintains an outstanding capacity retention of 84.5% even after 1700 cycles, demonstrating the feasibility of high-entropy doped Ni-rich cathodes when matched with a sulfide solid-state electrolyte. The application of high-entropy doping methodology for the development of advanced rechargeable batteries has been shown to provide a novel perspective on the improvement of the structural robustness and interfacial compatibility of Ni-rich cathode materials.
研究领域:
材料科学
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电化学
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储能技术
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锂离子电池
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固态电池
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DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Hui Zhang,Qiang Fu,Hongyun Qin,Xia Chen,Qicheng Zhang,Zixu Dong,Haoyuan Li,Shoudong Wang,Ming Wang
Hydrogen recovery from ammonia purge gas is a desirable method to relieve the pressure of increasing demand for hydrogen. Metal-organic frameworks (MOFs) are promising adsorbents for the separation of the H 2 –N 2 mixture. However, the separation of the H 2 –N 2 mixture using MOFs remains challenging due to the lack of adsorptive mechanism. Herein, the adsorption mechanism of the H 2 –N 2 mixture in SIFSIX-2-Cu-i has been systematically investigated with the method of a combination of excess adsorption experiments, molecular simulations , and DFT calculations. In the Grand Canonical Monte Carlo (GCMC) simulations, the polarizable force field was first applied to the adsorption of pure H 2 or N 2 and H 2 –N 2 mixture in SIFSIX-2-Cu-i. Ab Initio Molecular Dynamics (AIMD) was performed to investigate the distribution of the guest molecules in the pores of SIFSIX-2-Cu-i. Finally, Density functional theory (DFT) calculations were performed to predict the transfer of charge between MOF and guest molecules. Results revealed two binding sites of H 2 or N 2 in SIFSIX-2-Cu-i. A relatively high thermodynamic adsorption selectivity for N 2 over H 2 has been observed in SIFSIX-2-Cu-i. Furthermore, SIFSIX-2-Cu-i also exhibits a greater affinity with N 2 than with H 2 , which is probably because of the stronger induction interactions between F2 atoms and N 2 molecules. These findings are of significance to guide the design of the new highly selective adsorbents for the separation of H 2 /N 2 .
研究领域:
化学工程
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材料科学
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物理化学
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产品关联
DOI
高影响因子
FUEL
·
2020
·
IF 5.578
Limo He,Song Hu,Xiaofei Yin,Jun Xu,Hengda Han,Hanjian Li,Qiangqiang Ren,Sheng Su,Yi Wang,Jun Xiang
Fe-modified Ni/Al 2 O 3 catalysts with Fe/Ni molar ratios of 0, 0.5, 1 and 2 were prepared to promote the co-production of H 2 and carbon nanotubes (CNTs) during steam reforming of toluene as a tar model compound. After the addition of Fe, toluene conversion increased from 55.1% of Ni/Al 2 O 3 to 73.6% of F1N1A (Fe/Ni ratio of 1), and H 2 yield over F1N1A reached the maximum of more than 2000 mmol/(g-cata). Multi-walled carbon nanotubes with average diameter of 10–30 nm were generated and follow tip-growth mechanism. Compared with Ni/Al 2 O 3 , the addition of Fe remarkably increased the amount and quality of CNTs which had longer length and less tortuosity. These dual promoting effects on H 2 and CNTs after the addition of Fe were attributed to the strong interaction between Ni and Fe in Fe-Ni alloy. Fe-Ni alloy had the high activity for the decomposition performance of toluene and H 2 O to generate more H 2 and intermediates for improving the reforming reaction. Meanwhile, the high catalytic decomposition activity supplied more carbon species and the formation of Fe-Ni alloy enhanced the generation of metal carbide for promoting CNTs growth. Besides, the deposition of amorphous carbon was suppressed and the interaction between Ni particle and catalyst support was weakened after the addition of Fe, which kept the activity of catalyst and promoted the tip-growth of CNTs.
研究领域:
催化
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材料科学
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化学工程
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环境科学
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产品关联
DOI
高影响因子
ACS Applied Energy Materials
·
2021
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IF 6.024
Xinyao Zou,Chao Ma,Ang Li,Zhan Gao,Zulipiya Shadike,Kun Jiang,Junliang Zhang,Zhen Huang,Lei Zhu
Electrochemical conversion of CO2 to the syngas hybrid with the Fischer–Tropsch (FT) process is a promising way to produce synthetic fuels from renewable energy sources. The product distribution in liquid hydrocarbons produced by FT synthesis has strong dependence on the CO/H2 ratio of the syngas feedstock. Herein, we demonstrated the feasibility of tuning the CO/H2 ratio at a wide range by developing nanoparticle-assisted Ni–Co binary single-atom catalysts for electrocatalytic production of syngas. By controlling the elemental proportion of Ni–Co in the composite catalysts, electrochemical reduction of CO2 to syngas with a tunable CO/H2 ratio from 0.3 to 27.6 was achieved. For the binary catalysts with a Ni–Co ratio of 1:1, the CO/H2 ratio maintains at 1.3–1.5 in a broad potential range from −0.59 to −0.83 V versus reversible hydrogen electrode (RHE) and the total current density reaches ∼32.2 mA/cm2 at −1.0 V versus RHE. The promotion effect of nanoparticles on Ni–Co single-atom catalysts was validated by partial removal of nanoparticles and further density functional theory (DFT) calculations. As revealed by DFT calculations, nanoparticles incorporated in single-atom sites take essential roles in facilitating the adsorption of CO2 and the formation of *COOH. The origin of CO2RR and hydrogen evolution reaction reactivities can be identified as Ni–N4 and Co–N4 single-atom sites, respectively. The dual active sites allow the facile control of the CO/H2 ratio of electrochemical converted syngas, and it will be beneficial to downstream production of diverse chemicals.
研究领域:
催化
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电化学
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材料科学
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能源转换
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可持续化学
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产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
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IF 19
Jiawen Wang,Jinfu Wang,Zi Wang,Jiayue Wu,Jiaxuan Liao,Shenyuan Zhan,Xiaoye Chen,Xinhao Wang,Yongbao Wei,Qidong Zhou,Liefu Ye,Jinfeng Wu
Incontinence-associated dermatitis (IAD) leads to persistent tissue damage, antibiotic-resistant infections, and neurogenic inflammation, greatly impairing patients' quality of life. Current therapies fail to simultaneously eliminate resistant bacterial biofilms, neutralize alkaline conditions, and break the cycle of ammonia (NH 3 ) regeneration. Here, a piezoelectric gas therapy strategy based on platinum-decorated bismuth molybdate load in gelatin methacrylate (GelMA) hydrogel (Pt@BMO-Gel) is introduced. Under ultrasound excitation, Pt@BMO generates high piezoelectric potential to improve charge separation, selectively adsorbs NH 3 on BMO (001) crystal facets, efficiently degrades NH 3 to normalize pH, and enables sustained release of H 2 and NO for dual antibacterial and anti-inflammatory effects. Mechanistic insights from theoretical calculations show that the Pt (111) and BMO (001) surfaces lower energy barriers for H 2 formation and N─H bond cleavage, conducive to the generation of NO and H 2 . Transcriptomic profiling reveals downregulation of key nitrogen metabolism genes (arcC/hutH) in methicillin-resistant Staphylococcus aureus (MRSA) and disruption of the (p)ppGpp-mediated stringent response, effectively eradicating bacterial persistence via metabolic reprogramming. This study establishes Pt@BMO as an efficient piezoelectric catalyst for wound therapy, presenting a novel approach in medicine that transforms harmful NH 3 into therapeutic H 2 and NO, offering a promising treatment paradigm for infected wounds, such as incontinence-associated dermatitis.
研究领域:
生物医学工程
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伤口愈合
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抗菌治疗
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纳米医学
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压电材料
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气体治疗
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炎症性疾病
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产品关联
DOI
高影响因子
CATALYSIS TODAY
·
2022
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IF 6.562
Zhuangqing Wang,Xinchao Wang,Chao Zhang,Yinze Yang,Leilei Zhou,Haiyang Cheng,Fengyu Zhao
Catalytic conversion of furfural and its derivatives to value-added C 5 molecules has attractive much attention in the field of biomass conversion . In this paper, the selective hydrogenolysis of tetrahydrofurfuryl alcohol to 1,5-pentanediol has been studied over a series of PrO x promoted Ni/Al 2 O 3 catalysts. The catalytic performances and the promoting effects of PrO x , as well as the role of Ni and PrO x species have been discussed. The surface properties and structure of catalysts were examined by TEM, XRD, XPS, H 2 -TPR, H 2 -TPD, in-situ DRIFTS, etc. The presence of PrO x species promotes the reaction rate and changes product selectivity significantly, and a 79.2% 1,5-pentanediol selectivity can be obtained at 88.4% conversion over the NiPr 1.2 /Al 2 O 3 catalyst. The synergistic effect between defect-rich PrO x and the adjacent active Ni species has been confirmed to contribute to the superior catalytic performances. These results provide useful knowledge for the activation of cyclic ether bonds and the design of heterogeneous catalysts with lanthanide oxide supports.
研究领域:
催化
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生物质转化
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化学工程
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材料科学
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DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2023
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IF 9.5
Shuyue Pang,Yanhong Li,Xiaofang Chen,Aisheng Huang
The fabrication of mixed matrix membranes (MMMs) by intermixing suitable fillers with organic polymers is an effective strategy to surmount the well-known trade-off effect between gas permeability and selectivity, which can promote separation performance of membranes to a great extent. Two-dimensional (2D) metal-organic frameworks (MOFs) are considered as potential fillers for strengthening the separation performance of MMMs as they possess high aspect ratio and distinctive chemical characteristics. However, it remains challenging in engineering the morphology of the MOFs with desired pore structure and high aspect ratio. In this study, we firstly prepare c-axis oriented ZIF-95 sheets with lateral dimension exceeding 22 μm and thickness of around 3 μm by the solvothermal method. And then the ZIF-95 sheets are incorporated into the polyimide (PI) matrix to fabricate highly c -axis oriented ZIF-95@PI MMMs (denoted as COZIF-95@PI MMMs thereafter). Attributing to the straight permeation channel of ZIF-95 (3.6 Å) for gas permeation as well as its high compatibility with polyimide substrates, the COZIF-95@PI MMMs show a high gas separation capability. At 373 K and 100 kPa for the COZIF-95@PI MMM with 40 wt% loading, the mixture separation factors of H 2 /CH 4 and H 2 /CO 2 are 134 and 58, respectively, and the H 2 permeability exceeds 967 barrer , which is hopeful for the separation and purification of hydrogen.
研究领域:
材料科学
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化学工程
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膜技术
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产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2017
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IF 3.582
Yinghui Sun,Guojie Zhang,Jiwei Liu,Peiyu Zhao,Peng Hou,Ying Xu,Riguang Zhang
CH 4 CO 2 reforming to syngas was investigated over three different activated carbon catalysts. To better understand the influence of the supports on the catalytic properties , catalysts were analyzed by some characterization methods, such as nitrogen adsorption–desorption isotherms, XRD , H 2 -TPR, NH 3 -TPD, CO 2 -TPD, FTIR, TEM and EDX . The results showed that the catalyst with AC 2 as the support provided the best catalytic activity . The CH 4 conversion and CO 2 conversion were 92% and 98% at 900 °C, respectively; best selectivity with the H 2 /CO ratio was close to 1 among the three supports used. It also showed a better stability at 900 °C. H 2 -TPR analysis showed that Co species in Co/AC 2 catalyst were strong interaction with the support. It was observed that active metals were well dispersed on the AC 2 support by the TEM. In addition, the ratio of CH 4 /CO 2 also had great influence on the CH 4 and CO 2 conversion.
研究领域:
催化
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化学工程
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材料科学
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产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2020
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IF 3.573
Jincheng Mu,Jianfang Liu,Zhenzhen Ran,Muhammad Arif,Min Gao,Chen Wang,Shengfu Ji
MOF-808(Zr) with the coordinated unsaturated (CUS) Zr4+ centers was synthesized by the thermal reflux method, and a series of Au/MOF-808(Zr) catalysts with different Au loading percentages have been prepared by the impregnation–reduction method. The related X-ray diffraction, Fourier transform infrared spectroscopy, high-resolution transmission electron microscopy, X-ray photoelectron spectroscopy, N2 adsorption–desorption, Inductively coupled plasma-mass spectrometry, and NH3 temperature-programmed desorption characterizations have been undertaken to understand the structure of catalysts. The catalytic activity in CO2 with aniline/H2 to N-methylation and N-formylation has been studied in a batch reactor. Results show that the MOF-808(Zr) structures in catalysts are of high quality and damage-free. The Au nanoparticles (NPs) are highly dispersed on the surface of the MOF-808(Zr) cage with a mean size of 2–20 nm. Also, the catalysts could catalyze the conversion of CO2 with aniline/H2 to N-methylation and N-formylation products with a high efficiency. With a 3.0 wt % Au/MOF-808(Zr) catalyst, the conversion of aniline is 18.4%, and the selectivity of N-methylaniline is 80.9% and that of N,N-dimethylaniline is 19.1%. The preliminary reaction mechanism and the critical role of CUS were also studied. It is determined that H2 is adsorbed and activated on Au NPs. CO2 is adsorbed on the CUS Zr4+ acidic sites and O2– basic sites. The primary and secondary amines are adsorbed on the CUS Zr4+ acidic sites, where they react with CO2 and H2 to form N-formamide. Subsequently, N-formamide reacts with activated H2 to yield N-methylamine.
研究领域:
催化
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材料科学
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化学工程
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环境化学
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产品关联
DOI
高影响因子
Environmental Science-Nano
·
2022
·Vol. 9
·期 6
·1952-1960
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IF 9.473
Jiaqing He,Feng Gao,Haowei Wang,Fangyan Liu,Jiahui Lin,Biao Wang,Chuan Liu,Feng Huang,Zhang Lin,Mengye Wang
H2O2 is an environmentally friendly chemical for wide water treatments and H2 is regarded as an ideal substitute for traditional fossil energy. The industrial production of H2O2 is via the anthraquinone oxidation process, which, however, consumes extensive energy and produces pollution. Herein, based on the density functional theory (DFT) calculations, we report a green and sustainable piezocatalytic intermediate water splitting (IWS) process to simultaneously obtain H2O2 and H2 using C-doped KNbO3 nano single crystals as catalysts. The KNbO3 catalysts doped with suitable amounts of carbon show an enhanced water splitting rate, which could be attributed to the decreased reaction barriers on the C-KNbO3 surface and improved polarized built-in electric field, as evidenced by DFT simulations and PFM measurements. Remarkably, the piezocatalytic H2 evolution efficiency of 0.5 : 1 C-KNbO3 reaches 524.51 μmol g−1 h−1. Additionally, 0.5 : 1 C-KNbO3 could generate H2 and H2O2 simultaneously through two-electron piezocatalytic IWS reactions. This improved catalytic efficiency is attributed to the promoted piezo-response of KNbO3 after C doping, as revealed by PFM tests.
研究领域:
材料科学
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环境科学
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能源科学
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产品关联
DOI
高影响因子
JOURNAL OF POWER SOURCES
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2019
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IF 7.467
Qiulin Li,Heng Liu,Long-Cheng Zhang,Hao Chen,Hongjiu Zhu,Yuanke Wu,Maowen Xu,Shu-Juan Bao
Fe-N and pyridinic-N generally are considered the active sites of Fe-N-C catalyst. In this featured work, small uniform Fe/N-rich polymer spheres are selected to prepare the Fe-N-C catalyst and study how the sintering atmosphere (NH 3 , Ar, and H 2 ) to engineer their products. The findings reveal that the sintering atmosphere greatly affected not only the composition , aggregate state, and morphology of Fe, but also the graphitization degree and pore structure of carbon. In addition, XPS results suggest that Fe-N-C-NH 3 possesses the highest Fe-N and pyridinic-N content. Combining its abundant pores, high graphitization, and large specific surface area, the catalyst obtained in NH 3 atmosphere delivers best ORR catalytic performance (E 0 = 0.97 V, E 1/2 = 0.85 V vs RHE), which is even comparable to commercial Pt/C (E 0 = 0.97 V, E 1/2 = 0.83V vs RHE). Moreover, the catalyst exhibits greater stability and methanol resistance than those of Pt/C.
研究领域:
材料科学
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电化学
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产品关联
DOI
高影响因子
CERAMICS INTERNATIONAL
·
2024
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IF 5.1
Shuai Nie,Jing Li,Yunxia He,Xitao Yin
Gas sensors with the p–n heterojunction have demonstrated distinct sensing responses to reducing gases, yet a clear understanding of the reaction pathways and selective adsorption mechanisms for specific gas components remains elusive, impeding practical applications. In this study, we constructed an atomic-level NiO–In 2 O 3 heterojunction and explored its adsorption behaviors and sensing properties for CO and H 2 by first-principles calculations. Analysis of its electronic properties, focusing on binding energy, differential charge density, and density of states, confirmed the creation of a highly stable NiO–In 2 O 3 heterojunction and alterations in the coordination environment of the surface-active atoms. These changes potentially led to differences in the affinity between the gas molecules and the adsorption sites. The calculations of the adsorption properties revealed that the adsorption capacity of H 2 is relatively weak compared to the strong interactions between CO and heterojunction surface atoms, indicating a readily variable reaction pathway for H 2 . Consequently, the adsorption configuration at the interface site on the NiO–In 2 O 3 heterojunction surface exhibited a predominantly p-type response for CO and a unique n-type response for H 2 . This interfacial effect of the heterojunction is crucial for the selective adsorption of CO and H 2 . Furthermore, the opposite response signal was verified by gas sensing tests, which also presented the superior stability of the NiO–In 2 O 3 sensor. The p–n heterojunction of the corresponding composites was effectively characterized. This research offers new insights into the selective adsorption mechanism, paving the way for the development of gas sensors.
研究领域:
材料科学
·
传感器技术
·
理论计算
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）