CATALYSIS LETTERS
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2024
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IF 2.3
Li Ruili,Liu Lin,Ju Xiaohua,Feng Ji,Wang Jiemin,Guo Jiangping,He Teng,Chen Ping
The essential role of metal–support interaction in ammonia synthesis was investigated by using a Pr 6 O 11 supported Ru nanoparticles (NPs) catalyst system. Loading of Ru NPs onto the Pr 6 O 11 support with relatively low surface area yields similar metal dispersion with respect to conventional SiO 2 support. The Ru NPs on the Pr 6 O 11 was found to exhibit excellent catalytic performance in ammonia synthesis, superior to free-standing Ru NPs and Ru NPs on conventional SiO 2 support. Detailed structure analysis results reveal that the superior activity of Ru/Pr 6 O 11 can be attributed to the enhanced interaction between the Ru NPs and Pr 6 O 11 , which can modulate the electronic structure of Ru NPs and trigger catalytic ammonia synthesis over Ru NPs on Pr 6 O 11 . Furthermore, nitrogen isotope exchange experiment reveals that superior nitrogen dissociation ability is essential for the excellent activity and intrinsic activity of Ru/Pr 6 O 11 in ammonia synthesis. These findings demonstrate that Pr 6 O 11 can be used as a new kind of support for preparation of efficient Ru-based catalysts for ammonia synthesis, and also open up opportunities for design of Pr 6 O 11 supported metal catalysts for other catalytic reactions. Graphitical Abstract Interaction between the Ru NPs and Pr 6 O 11 can modulate the electronic structure of Ru NPs and trigger catalytic ammonia synthesis over Ru NPs on Pr 6 O 11 .
研究领域:
催化化学
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材料科学
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物理化学
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DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
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2016
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IF 2.628
Xinping Duan,Yan Yin,Xuelin Tian,Jinhuo Ke,Zhaojun Wen,Jianwei Zheng,Menglin Hu,Linmin Ye,Youzhu Yuan
Disintegration or redispersion of supported sintered gold nanoparticles (Au NPs) in the presence of alkyl halide can give catalyst regeneration or redispersion of sintered Au catalysts. The selectivity of alkyl halides, temperature and size distributions were investigated to elucidate the redispersion of Au NPs during halide-induced decomposition. This study proved that the alkyl halide induced the redispersion of sintered Au NPs which depended on the R–X (X = I, Br, Cl) bond dissociation energy (BDE) and thus provided a simple descriptor for the regeneration of inactive supported Au catalysts. A correlation between the BDE of R–X and dispersion efficiency was established. The tendency for disintegration and redispersion followed the R–X BDE of the alkyl halide. Compared to alkyl chlorides and bromides, iodides were more efficient for redispersing sintered Au NPs. As a descriptor, the BDE of R–I played a crucial role in particle redispersion. These findings provided insights into the mechanism of organic halide-induced Au NP disintegration and the effect of the halide type on the redispersion of sintered catalysts.
研究领域:
化学
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催化科学
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产品关联
DOI
高影响因子
FUEL
·
2023
·
IF 7.4
Guang-Hui Liu,Yong-Chao Qi,Han Wang,Ai-Min Wang,Yu-Hong Kang,Yong Gao,Ni Bai,Zhan-Ku Li,Xian-Yong Wei
This paper focused on the complementary advantages of density functional theory (DFT) calculation and catalytic reaction regulation. Based on the effective identification of intermediates, the possible catalytic hydroconversion (CHC) pathways of lignite-derived aryl ethers over Ni/mordenite were discussed. Bond dissociation energy (BDE) calculations of >C–O– bonds in different substrates and intermediates show that BDEs of >C ar –O– bonds are generally higher than those of >C al –O– bonds, and there is obvious electron aggregation near O atoms. Mulliken charge distribution analyses of different atomic sites further revealed the possible adsorption sites of active hydrogen, especially H · and H + . Possible cleavage pathways were further speculated by evaluating the stability of different leaving groups. In the early stage of CHC, aromatic ring hydrogenation and >C al –O– bond cleavage dominate, rather than >C ar –O– bond cleavage. Enthalpy change analyses combined with the CHC of real substrates further indicate that lowering temperature is beneficial to the cleavage of >C ar –O– bonds under the premise of inhibiting H ··· H transfer and obtaining H · effectively. Appropriately increasing the support acidity to ensure sufficient H + release is conducive to >C al –O– bond cleavage, especially direct dehydroxylation/dehydration. The analysis of synergetic transfer pathways of active hydrogen during the CHC provides theoretical guidance for the pathway optimization of converting lignite into high-quality clean liquid fuels.
研究领域:
化学工程
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能源科学
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产品关联
DOI
高影响因子
Advanced Powder Materials
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2024
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IF 28.6
Jingjing Yan,Rundong Wu,Guoqiang Jin,Litao Jia,Gang Feng,Xili Tong
Water electrolysis via alkaline hydrogen evolution reaction (HER) is a promising approach for large-scale production of high-purity hydrogen at a low cost, utilizing renewable and clean energy. However, the sluggish kinetics derived from the high energy barrier of water dissociation impedes seriously its practical application. Herein, a series of hybrid Pt nanoclusters/Ru nanowires (Pt/Ru NWs) catalysts are demonstrated to accelerate alkaline HER. And the optimized Pt/Ru NWs (10 % wt Pt) exhibits exceptional performance with an ultralow overpotential (24 mV at 10 mA cm −2 ), a small Tafel slope (26.3 mV dec −1 ), and long-term stability, outperforming the benchmark commercial Pt/C-JM-20 % wt catalyst. This amazing performance also occurred in the alkaline anion-exchange membrane water electrolysis devices, where it delivered a cell voltage of about 1.9 V at 1 A cm −2 and an outstanding stability (more than 100 h). The calculations have revealed such a superior performance exhibited by Pt/Ru NWs stems from the formed heterointerfaces, which significantly reduce the energy barrier of the decisive rate step of water dissociation via cooperative-action between Pt cluster and Ru substance. This work provides valuable perspectives for designing advanced materials toward alkaline HER and beyond.
研究领域:
材料科学
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催化化学
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可再生能源
✓ 已验证
产品关联
DOI
高影响因子
Science Advances
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2019
·Vol. 5
·期 8
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IF 12.804
Yuequn Shang,Yuan Liao,Qi Wei,Ziyu Wang,Bo Xiang,Youqi Ke,Weimin Liu,Zhijun Ning
Organic-inorganic hybrid halide perovskites are emerging as promising materials for next-generation light-emitting diodes (LEDs). However, the poor stability of these materials has been the main obstacle challenging their application. Here, we performed first-principles calculations, revealing that the molecule dissociation energy of Dion-Jacobson (DJ) structure using 1,4-bis(aminomethyl)benzene molecules as bridging ligands is two times higher than the typical Ruddlesden-Popper (RP) structure based on phenylethylammonium ligands. Accordingly, LEDs based on the DJ structure show a half-lifetime over 100 hours, which is almost two orders of magnitude longer compared with those based on RP structural quasi–two-dimensional perovskite. To the best of our knowledge, this is the longest lifetime reported for all organic-inorganic hybrid perovskites operating at the current density, giving the highest external quantum efficiency (EQE) value. In situ tracking of the film composition in operation indicates that the DJ structure was maintained well after continuous operation under an electric field.
研究领域:
材料科学
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物理学
✓ 已验证
DOI
高影响因子
ADVANCED MATERIALS
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2024
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IF 27.4
Hongliang Li,Jingyang Wang,Sheng Xu,Aoyuan Chen,Hangyu Lu,Yan Jin,Shaohua Guo,Jia Zhu
Na-ion batteries (NIBs) are sustainable alternatives to Li-ion technologies due to the abundant and widely-distributed resources. However, the most promising cathode materials of NIBs so far, O3 layered oxides, suffer from serious air instability issues, which significantly increases the manufactural cost and carbon footprint because of the long-term use of dry rooms. While some feasible strategies are proposed via case studies, universal design strategies for air-stable cathodes are yet to be established. Herein, the air degradation mechanisms of O3 cathodes are investigated via combined first-principles and experimental approaches, with bond dissociation energy proposed as an effective descriptor for predicting air stability. Experimental validations in various unary, binary, and ternary O3 cathodes confirm that the air stability can indeed be effectively improved via simple compositional design. Guided by the predictive model, the designed material can sustain 30-day air-storage without structural or electrochemical degradation. It is calculated that such air-stable cathodes can significantly reduce both energy consumption (≈4 100 000 kWh) and carbon footprint (≈2200-ton CO 2 ) annually for a 2 GWh NIBs manufactory. Therefore, the fundamental understandings and universal design strategy presented open an avenue for rational materials design of NIBs toward both elemental and manufactural sustainability.
研究领域:
材料科学
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能源存储
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可持续技术
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电化学
✓ 已验证
DOI
高影响因子
JOURNAL OF THE ENERGY INSTITUTE
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2025
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IF 6.2
Jinrui Guo,Yaozong Duan,Fashe Li,Huicong Zhang,Fangguan Tan,Xinhua Qian,Hua Wang
In this study, the emission characteristics and formation mechanisms of aldehydes from biodiesel combustion, both before and after oxidation, are comprehensively investigated through Bunsen burner experiments coupled with Chemkin and Gaussian software simulations. The results reveal that the aldehyde concentration initially decreases, then increases, and eventually decreases again as the oxidation time of the original biodiesel increases. During the first 0–6 h of biodiesel oxidation, its overall saturation increases, while the aldehyde generation potential decreases. After 8 h, oxidation products with low bond dissociation energy (BDE) and multiple double bonds readily dissociate into aldehyde intermediates, such as CH 3 O, CH 2 CHO, and C 4 H 6 . This causes an increase in the concentrations of formaldehyde and acetaldehyde by 120.2 % and 188.3 %, respectively. Between 10 and 12 h, the oxidation products undergo transformation, significantly reducing aldehyde emissions. As the overall carbon chain length of biodiesel shortens, combustion accelerates, and the aldehyde peaks rise more rapidly, appearing earlier. The lowest BDE values, both before and after biodiesel oxidation, are concentrated near the ester group and C=C bond. The oxidation product methyl alpha-eleostearate exhibits the lowest BDE of 315.67 kJ/mol. The formation of oxidation products of biodiesel like methyl alpha-eleostearate leads to incomplete combustion, with aldehyde emissions increasing by 9.5–183.2 %. This is due to the electron-withdrawing, electronegative, and resonance effects of the double bonds, which lower the energy required for H-abstraction and β-decomposition reactions during aldehyde formation.
研究领域:
环境科学
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化学工程
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燃烧技术
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计算化学
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能源研究
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
·
IF 9.7
Min Li,Sheng-Xia Yang,Yu-Feng Liu,Ya-Nan Zhou,Hai-Jun Liu,Xin-Yu Zhang,Bin Dong,Qun-Wei Tang
The hydrogen evolution reaction (HER) process of metal hydroxides is significantly limited by weak hydrogen adsorption and requires a large overpotential. This study presents coordination engineering strategy to activate inert copper hydroxide through the introduction of stoichiometric nitrate ligands (CuHN). Nitrate and Cu are coordinated in an atomic ratio of 1 to 2, leading to expanded lattice space compared to conventional Cu hydroxide. This modification facilitated the successful doping of numerous Co atoms to synthesize the Co-CuHN sample, which works synergistically with nitrate to enhance HER activity. Experimental and theoretical analyses demonstrate that nitrate and Co provide electrons to Cu, thereby modulating the d-band center and surface adsorption capability. Compared to Cu(OH) 2 , Co-CuHN exhibits a reduced water dissociation energy barrier of 0.54 eV, supplying abundant protons for hydrogen generation. Notably, the Gibbs free energy of hydrogen adsorption is optimized to approach zero. Consequently, Co-CuHN demonstrates a small Tafel slope of 40.0 mV dec −1 and requires a low overpotential of 18 mV (10 mA cm −2 ), which is 99 mV lower than control Cu(OH) 2 . This work is expected to provide a deeper understanding of anion coordination regulation of copper hydroxide.
研究领域:
电化学
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材料科学
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催化
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纳米技术
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能量转换
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2025
·
IF 13.2
Liancen Li,Guangfu Qian,Litao Ge,Yunpeng Wang,Xinyu Cao,Jiawei Li,Douyong Min,Jinli Chen,Panagiotis Tsiakaras
Biomass-derived carbon-based electrocatalysts often suffer from low performance in hydrogen evolution reaction (HER) at high current density, limiting their industrial use. Herein, a Mn 2 Mo 3 O 8 -Ni heterojunction is integrated into a self-supported lignin-derived carbon framework on nickel foam (LC-Mn 2 Mo 3 O 8 @Ni/NF) to enhance HER performance. Electrochemical tests demonstrate that LC-Mn 2 Mo 3 O 8 @Ni/NF exhibits effective HER activity under pH-universal conditions (Alkali: E -10/−2000 = −54.7/322.9 mV; Acidic: E -10/−2000 = −39.5/431.5 mV; Neutral: E -10/−600 = −84.2/421.9 mV). Density functional theory calculations reveal that the synergy of lignin-derived carbon and the heterojunction redistributes electrons, creating an electron-rich carbon layer and electron-deficient Mn 2 Mo 3 O 8 @Ni, increasing active sites. The optimized d -band center enhances *H adsorption/desorption (ΔG ⁎H = −0.12 eV) and lowers the water dissociation energy (0.61 eV), facilitating the Volmer step and boosting HER activity across all pH conditions. Furthermore, LC-Mn 2 Mo 3 O 8 @Ni/NF maintains stability at −500 mA cm −2 for 140 h without significant performance loss, attributed to its super-hydrophilic, gas-repellent properties, and corrosion-resistant porous self-supported lignin-derived carbon, thus facilitating HER across pH-universal conditions. This research provides an efficient catalyst for HER and offers valuable insight for developing high-performance biomass-derived carbon-based electrocatalysts for water electrolysis.
研究领域:
电化学
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材料科学
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催化
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纳米技术
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能量转换
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计算化学
✓ 已验证
DOI
高影响因子
Nature Communications
·
2022
·Vol. 13
·期 1
·1-10
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IF 17.694
Li Yinghao,Peng Chun-Kuo,Hu Huimin,Chen San-Yuan,Choi Jin-Ho,Lin Yan-Gu,Lee Jong-Min
Developing high-performance electrocatalysts for hydrogen evolution reaction (HER) is crucial for sustainable hydrogen production, yet still challenging. Here, we report boron-modulated osmium (B-Os) aerogels with rich defects and ultra-fine diameter as a pH-universal HER electrocatalyst. The catalyst shows the small overpotentials of 12, 19, and 33 mV at a current density of 10 mA cm −2 in acidic, alkaline, and neutral electrolytes, respectively, as well as excellent stability, surpassing commercial Pt/C. Operando X-ray absorption spectroscopy shows that interventional interstitial B atoms can optimize the electron structure of B-Os aerogels and stabilize Os as active sites in an electron-deficient state under realistic working conditions, and simultaneously reveals the HER catalytic mechanisms of B-Os aerogels in pH-universal electrolytes. The density functional theory calculations also indicate introducing B atoms can tailor the electronic structure of Os, resulting in the reduced water dissociation energy and the improved adsorption/desorption behavior of hydrogen, which synergistically accelerate HER.
研究领域:
材料科学
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电化学
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催化
·
可持续能源
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
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2025
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IF 7.3
Ge-liang Xie,Yang Cao,Sheng-ren Li,Qian-qian Lu,Wei Chen,Shuai Gao,Wei Qiu,Chao He,Zhen Fang,Lujiang Xu
Lignin valorization through catalytic upgrading to nitrogen-containing aromatics represents a critical pathway for sustainable chemical production. Using vanillin, a key lignin depolymerization product, as a platform molecule, we demonstrate the first integrated strategy combining cyanide-free cyanation and gas-phase hydrodeoxygenation (HDO) to synthesize hydroxybenzonitriles (HBNs). Bond dissociation energy (BDE) analysis revealed the cyano group’s selective retention (C≡N: 136.21 kcal/mol vs C–O: 62.44–116.17 kcal/mol), guiding targeted HDO pathway design. A green H2O/HCOOH system achieved 99.2 mol % vanillonitrile yield under mild conditions (85 °C, 12 h), surpassing conventional DMF-based methods. Engineered Mo/TiO2 catalysts with triple functional sites (oxygen vacancies, suitable content of Mo5+, strong metal–support interaction) achieved 57.6% HBN yield in continuous gas-phase HDO, outperforming Mo/ZrO2. The catalyst retained 90% of its initial activity over eight cycles due to enhanced metal–support interactions. This work establishes a sustainable route for lignin-to-chemical conversion, advancing catalyst design principles for biomass upgrading.
研究领域:
催化
·
绿色化学
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生物质转化
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有机合成
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
·
IF 9.4
Yujie Zhang,Xin He,Haomiao Li,Wenjie Zhao,Kangli Wang,Kai Jiang
Rechargeable magnesium battery is regarded as the promising candidate for the next generation of high-specific-energy storage systems. Nevertheless, issues related to severe Mg-Cl dissociation at the electrolyte–electrode interface impede the insertion of Mg 2+ into most materials, leading to severe polarization and low utilization of Mg-storage electrodes. In this study, a metal–organic polymer (MOP) Ni-TABQ (Ni-coordinated tetramino-benzoquinone) with superior surface catalytic activity is proposed to achieve the high-capacity Mg-MOP battery . The layered Ni-TABQ cathode, featuring a unique 2D π-d linear conjugated structure, effectively reduces the dissociation energy of Mg x Cl y clusters at the Janus interface, thereby facilitating Mg 2+ insertion. Due to the high utilization of active sites, Ni-TABQ achieves high capacities of 410 mAh/g at 200 mA g −1 , attributable to a four-electron redox process involving two redox centers, benzoid carbonyls, and imines . This research highlights the importance of surface electrochemical processes in rechargeable magnesium batteries and paves the way for future development in multivalent metal-ion batteries.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）