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Catalysts · 2022 ·Vol. 12 ·期 4 ·426 · IF 4.501

Boosted Catalytic Activity toward the Hydrolysis of Ammonia Borane by Mixing Co- and Cu-Based Catalysts

Jinyun Liao,Yujie Wu,Yufa Feng,Haotao Hu,Lixuan Zhang,Jingchun Qiu,Junhao Li,Quanbing Liu,Hao Li

Promoting the activity of heterogeneous catalysts in the hydrolysis of ammonia borane for hydrogen production is still a challenging topic for researchers in the hydrogen energy and catalysis fields. Herein, we present a universal, simple and efficient strategy to boost the catalytic performance toward AB hydrolysis by mixing Co- and Cu-based catalysts for the first time. Synergistic catalysts with remarkably enhanced activity can be obtained by mixing a Co-based catalyst and a Cu-based catalyst together, such as Co3O4and Cu3(MoO4)2(OH)2, Co3O4and Cu3(PO4)2,Co3(PO4)2and Cu3(MoO4)2(OH)2, Co3(PO4)2and Cu3(PO4)2, and CuO and Co3O4. For example, the turnover frequency (TOF) for the mixture catalyst of Co3O4and Cu3(MoO4)2(OH)2with a mass ratio of 4:1 is up to 77.3 min−1, which is approximately 11.5 times higher than that of the sum of Co3O4and Cu3(MoO4)2(OH)2. The reasons for these findings are discussed in detail. The observations and conclusions in this work may provide a guideline for promoting the hydrolysis of ammonia borane through a simple and effective approach.

研究领域: 氢能领域 · 催化化学
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Catalysts · 2020 ·Vol. 10 ·期 12 ·1455 · IF 3.52

Synthesis and Characterization of Amorphous Molybdenum Sulfide (MoSx)/CdIn2S4 Composite Photocatalyst: Co-Catalyst Using in the Hydrogen Evolution Reaction

Qi Li,Wanli Liu,Xuejian Xie,Xianglong Yang,Xiufang Chen,Xiangang Xu

Co-catalyst deposition is used to improve the surface and electrical properties of photocatalysts. In this work, MoSx/CdIn2S4nanocomposites were prepared by a facile hydrothermal and photodeposition route. The basic crystalline phases and morphology of the as-prepared samples were determined, and these results showed that MoSxwas tightly anchored onto CdIn2S4by sharing the same S atom. In the hydrogen production experiments, MoSx/CdIn2S4-40 displayed the optimal photocatalytic hydrogen production yield in 4 h. The H2evolution rate reached 2846.73 μmol/g/h, which was 13.6-times higher than that of pure CdIn2S4. Analyzing the photocatalytic enhancement mechanisms revealed that this unique structure had a remarkable photogenerated electron-hole pair separation efficiency, rapid charge carrier transfer channels, and more abundant surface reaction sites. The use of co-catalyst (MoSx) greatly improved the photocatalytic activity of CdIn2S4.Keywords:co-catalyst;photocatalyst;hydrogen production;CdIn2S4;MoSx

研究领域: 材料科学 · 能源科学
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INORGANICA CHIMICA ACTA · 2025 · IF 3.2

Study on the catalytic performance and kinetics of ethylene oligomerization catalyzed by Salicylaldiminato Phthalocyanine nickel catalyst

Na Zhang,Xiaoyue Wang,Sen Shen,Guohui Qi,Liduo Chen,Cuiqin Li,Jun Wang

A novel salicylaldiminato phthalocyanine nickel catalyst was prepared and characterized by FT-IR, UV–Vis, 1 H NMR, ICP-MS, TG-DSC and elemental analysis. The catalytic performance of ethylene oligomerization catalyzed by salicylaldiminato phthalocyanine nickel catalyst was investigated. The catalytic activity could reach up to 1.25  ×  10 6  g (mol Ni·h) −1 , and the products were mainly butene, hexene as well as a small amount of octene when the cyclohexane was used as solvent, the MAO was used as co-catalyst. In addition, the kinetics of ethylene oligomerization was also investigated. The kinetic parameters such as the reaction order to the nickel molar concentration ( n ) and oligomerization pressure ( m ), the apparent activation energy ( E a) and the pre-exponential factor (A) were determined. The result indicated that the reaction order to the nickel molar concentration was 1.18, the reaction order to oligomerization pressure was 1.12, and the apparent activation energy was 54.78 kJ/mol when the nickel concentration was 5 μmol/L, the oligomerization pressure was 1.0 MPa, and the oligomerization temperature was 5–35 °C.

CAS / MDL: 90-02-8
研究领域: 化学工程 · 催化科学
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CHINESE JOURNAL OF CATALYSIS · 2023 · IF 16.5

Atomically dispersed Ni-N-C catalyst derived from NiZn layered double hydroxides for efficient electrochemical CO2 reduction

Ping Zhang,Hao Chen,Lin Chen,Ying Xiong,Ziqi Sun,Haoyu Yang,Yingke Fu,Yaping Zhang,Ting Liao,Fei Li

Atomically dispersed catalytic metal sites anchored on N-doped carbon support catalysts (M-N-C) show great prospects for CO 2 electroreduction. Here, single-layer NiZn layered double hydroxides (NiZn-LDHs) was used as a sacrificial assistant to fabricate single-Ni atom anchored on ultrathin porous carbon catalyst. NiZn-LDHs were exfoliated to single-layer by polyhydroxy compounds which took as the carbon resource in Ni-N-C, and single layer NiZn LDHs taking as the Ni resource could avoid the agglomeration of Ni atoms during calcining. The CO Faradaic efficiency (FE CO ) of the synthesized Ni-N-C catalyst exceeded 90% at −0.6 to −1.0 V and a FE CO of 95.2% with a current density of 24 mA cm −2 at −0.9 V. This work not only provides a new method for preparing M-N-C catalysts, but also offers an effective and controllable strategy for large-scale production of high-performance single-atom catalysts.

CAS / MDL: 298-14-6
研究领域: 材料科学 · 催化化学 · 环境科学
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JOURNAL OF ALLOYS AND COMPOUNDS · 2024 · IF 5.8

Mechanistic investigation of ammonia adsorption and reforming over Ni, Ru loaded catalysts toward green H2 production of marine engines: DFT calculation and experimental evaluation

Yi Zhang,Gesheng Li,Zunhua Zhang,Yong Huang,Minghao Li,Jian Li,Mengni Zhou

Highly active catalysts suitable for ammonia reforming reactions have been comprehensively investigated by density functional theory (DFT) calculations and experimental tests. Non-precious metal Ni, precious metal Ru and Ru-Ni composite metal are selected as catalytic activity surfaces, and a series of three-dimensional metal-packed catalyst models are constructed parallelly. Then, to elucidate the rate-determining step of reforming reaction, in-depth analysis of microscopic reaction mechanisms for amino groups (including H and NH x , x =0–3) adsorption, dissociation, recombination and desorption are carried out by simulation parameters and experimental data. The results indicate that NH 3 exhibits highly stable adsorption configurations (Bridge site) on both Ni, Ru-based catalyst surfaces , with the adsorption position having a relatively minor effect on adsorption energy . It is worth noting that Ni-based catalyst exhibits better adsorption behaviors towards NH 3 compared to Ru. Whereas, during stepwise dehydrogenation of NH 3 and subsequent N 2 and H 2 recombination and desorption processes, the reaction energy barriers confirm experimental observations of higher activity displayed by Ru-based catalyst in low-temperature range of 400–500 °C. Interestingly, N 2 synthesis behavior of innovative Ru-Ni bimetallic tandem catalyst surface possesses the lowest reaction energy barrier than other models, which is attributed to the adsorption capability of Ni layers and the catalytic activity of Ru atoms. The experimental results also demonstrate that under typical engine exhaust conditions, the H 2 production efficiency of 1 %Ru-3 %Ni/Al 2 O 3 surpasses that of 1 %Ru/Al 2 O 3 by 6.2 %, showcasing exceptional stability.

CAS / MDL: 13478-00-7 14898-67-0
研究领域: 催化化学 · 能源材料 · 理论计算化学
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INORGANIC CHEMISTRY COMMUNICATIONS · 2024 · IF 4.4

Solvent-free oxidation of alcohols by a heterogeneous Fe3O4@SiO2-DTPA-Ru nanocatalyst

Haijiao Jia,Xinyu Xu,Yuchen Cui,Mengqi Cheng,Guirong Borjihan,Xiao Zhang,Shengbo Yang,Youxin Li

A novel magnetic heterogeneous ruthenium catalyst (Fe 3 O 4 @SiO 2 -DTPA-Ru) was prepared by using magnetic silicon spheres as support, ethylenediaminepentaacetic acid (DTPA) as functional ligands, ruthenium chloride as catalyst precursor. The results obtained after a series of characterizations showed that the catalyst Fe 3 O 4 @SiO 2 -DTPA-Ru was 5–15 nm in size with a 0.205 nm lattice and contained 0.31 mmol Ru/g catalyst. It also had a good thermal stability under 232°C which was verified by thermal filtration method. Besides, the saturation magnetic intensity was as high as 20.54 emu/g. The catalyst Fe 3 O 4 @SiO 2 -DTPA-Ru was applied for the first time into thirteen oxidation reactions of aromatic alcohols and showed good catalytic activity even the yields of eleven aromatic alcohols were all over 90%. In catalyzing 1-phenylethanol to acetophenone, its TOF and TON were 9677 h −1 and 6991, respectively. The Fe 3 O 4 @SiO 2 -DTPA-Ru catalyst could still maintain good reusability and catalytic performance after 15 cycles of 1-phenylethanol oxidation, which was superior to many reported catalysts and had great potential in future industrial production.

CAS / MDL: 75-05-8 67-56-1
研究领域: 化学 · 催化材料科学
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2025 · IF 21.1

Charge regulation through rare earth metal oxides for single-atomic/cluster Co-based electrocatalysts towards boosting oxygen reduction reaction

Shufan Wang,Lingfei Li,Yun Zheng,Chenhui Xu,Zewen Zhuang,Kaian Sun,Wei Yan,Jiujun Zhang

Single-atomic/cluster metal-based electrocatalysts (M-N-C) is one of the most promising non-noble metal catalysts for the oxygen reduction reaction (ORR), but their practical application is severely hindered by insufficient activity and durability. Herein, charge regulation through rare earth metal oxides (REMOs) for single-atomic/cluster metal based electrocatalysts is proposed for boosting ORR, in which the Co-based catalyst is taken as a representative considering its typicality and universality, and CeO 2 is selected as representative after systematic computational screening from more than 10 types of REMOs. As a result, a novel REMO-tailored M-N-C electrocatalyst (REMO-Co-N-C) has been successfully achieved, which demonstrates a remarkably increased activity and superior durability, namely a half-wave potential (E₁/₂) of 0.90 V and only a loss of 8 mV (E₁/₂) after 10,000 cycles. Moreover, in-situ experiments and matched theoretical simulations come together organically to clearly and directly reveal the origin and catalytic behavior of the proposed electrocatalysts. Namely the charge regulation through REMO for M-N-C can effectively modify the electronic structure of the M sites, accelerate the reaction rate, and enhance OH* desorption. This work offers a new insight for promoting M-N-C catalysts through REMO tailoring, that beyond the conventional use of d-block and p-block elements.

研究领域: 材料科学 · 电化学 · 催化科学
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Catalysts · 2022 ·Vol. 12 ·期 9 ·998 · IF 4.501

Well-Defined Ultrasmall V-NiP2 Nanoparticles Anchored g-C3N4 Nanosheets as Highly Efficient Visible-Light-Driven Photocatalysts for H2 Evolution

Mengfan Niu,Liyun Cao,Qianqian Liu,Xiaoyi Li,Qian Chen,Dinghan Liu,Wenbin Li,Jianfeng Huang,Liangliang Feng

Exploring low-cost and highly active, cost-effective cocatalysts is of great significance to improve the hydrogen evolution performance of semiconductor photocatalysts. Herein, a novel ultrasmall V-doped NiP2nanoparticle, as an efficient cocatalyst, is reported to largely upgrade the photocatalytic hydrogen evolution reaction (HER) of g-C3N4nanosheets under visible-light irradiation. Experimental results demonstrate that V-NiP2cocatalyst can enhance the visible-light absorption ability, facilitate the separation of photo-generated electron-hole pairs and boost the transfer ability of electrons of g-C3N4. Moreover, the V-NiP2/g-C3N4hybrid exhibits prominent photocatalytic HER activity 17 times higher than the pristine g-C3N4counterpart, even outperforming the 1 wt.% platinum-loaded g-C3N4. This work displays that noble-metal-free V-NiP2cocatalyst can serve as a promising and efficient alternative to Pt for high-efficiency photocatalytic H2evolution.Keywords:g-C3N4;cocatalyst;V-NiP2;photocatalyst;hydrogen evolution reaction

研究领域: 材料科学 · 催化化学
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RSC Advances · 2017 ·Vol. 7 ·期 84 ·53622-53630 · IF 3.108

The recycle of red mud as excellent SCR catalyst for removal of NOx

Changming Li,Hong Zeng,Pingle Liu,Jian Yu,Feng Guo,Guangwen Xu,Zhan-guo Zhang

The development of new routes for the utilization of red mud (RM) waste is very urgent due to its huge accumulation and potential environmental harm. By taking advantage of its Fe–Al–Si–Ti composition and excellent plasticity, we developed a ball milling and acid–base neutralization method to reuse the RM waste as Fe-based denitration catalysts. The resulting RM catalysts demonstrate excellent catalytic activity and stability with >90% NO conversion above 400 °C in the presence of SO2 and H2O, which is even much better than that of a commercial V–W–Ti catalyst. Characterization data reveal that our treatment eliminates poisonous alkaline metal elements and increases dispersion of RM particles, making the RM active for denitration reactions. The formation of ferric sulfate species with more reducible Fe3+/Fe2+ active sites by a SO2 activation method can further enhance the denitration activity. Moreover, NH3-TPD and in situ IR results demonstrate that the NH3-SCR reaction over the RM catalyst follows the Eley–Rideal mechanism at high temperature and the increased absorption of NH3 for alkaline metal-eliminated or SO2-activated samples accounts for its high DeNOx efficiency. The demonstrated feasibility for reusage of the RM as DeNOx catalyst has promising industrial prospects for its extremely low cost, no toxicity, and high efficiency.

研究领域: 环境科学 · 催化化学
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CHINESE JOURNAL OF CATALYSIS · 2025 · IF 17.7

Size-dependent strong metal-support interaction modulation of Pt/CoFe2O4 catalysts

Yangyang Li,Jingyi Yang,Botao Qiao,Tao Zhang

Supported metal catalysts are the backbone of heterogeneous catalysis, playing a crucial role in the modern chemical industry. Metal-support interactions (MSIs) are known important in determining the catalytic performance of supported metal catalysts. This is particularly true for single-atom catalysts (SACs) and pseudo-single-atom catalysts (pseudo-SACs), where all metal atoms are dispersed on, and interact directly with the support. Consequently, the MSI of SACs and pseudo-SACs are theoretically more sensitive to modulation compared to that of traditional nanoparticle catalysts. In this work, we experimentally demonstrated this hypothesis by an observed size-dependent MSI modulation. We fabricated CoFe 2 O 4 supported Pt pseudo-SACs and nanoparticle catalysts, followed by a straightforward water treatment process. It was found that the covalent strong metal-support interaction (CMSI) in pseudo-SACs can be weakened, leading to a significant activity improvement in methane combustion reaction. This finding aligns with our recent observation of CoFe 2 O 4 supported Pt SACs. By contrast, the MSI in Pt nanoparticle catalyst was barely affected by the water treatment, giving rise to almost unchanged catalytic performance. This work highlights the critical role of metal size in determining the MSI modulation, offering a novel strategy for tuning the catalytic performance of SACs and pseudo-SACs by fine-tuning their MSIs.

研究领域: 催化化学 · 材料科学
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2021 · IF 5.816

Catalyst support effect on ammonia decomposition over Ni/MgAl2O4 towards hydrogen production

Yu Qiu,Enkang Fu,Feng Gong,Rui Xiao

Ammonia is a prospective fuel for hydrogen storage and production, but its application is limited by the high cost of the catalysts (Ru, etc. ) to decompose NH 3 . Decomposing ammonia using non-precious Ni as catalysts can therefore improve its prospects to produce hydrogen. This work proposes several Ni/MgAl 2 O 4 with the support properties tuned and investigates the support effect on the catalytic performance. Ni/MgAl 2 O 4 -LDH shows high NH 3 conversion (∼88.7%) and H 2 production rate (∼1782.6 mmol g −1  h −1 ) at 30,000 L. kg −1  h −1 and 600 °C, which is 1.68 times as large as that of Ni/MgAl 2 O 4 -MM. The performance remains stable over 30 h. The characterizations manifest that the high specific surface area of Ni/MgAl 2 O 4 -LDH can introduce highly dispersed Ni on the surface. Kinetics analysis implies promoted NH 3 decomposition reaction and alleviated H 2 poisoning for Ni/MgAl 2 O 4 -LDH. A roughly linear relationship is obtained by fitting the curves of dispersed Ni on the surface vs the reaction orders regarding H 2 and NH 3 . This indicates that enhanced NH 3 decomposition performance can be ascribed to the strengthened NH 3 decomposition reaction and weakened H 2 poisoning by the highly dispersed Ni on the MgAl 2 O 4 -LDH surface. This work provides an opportunity to develop highly active and cost-effective catalysts to produce hydrogen via NH 3 decomposition.

研究领域: 化学工程 · 能源科学
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2023 · IF 22.1

Cu-supported nano-ZrZnOx as a highly active inverse catalyst for low temperature methanol synthesis from CO2 hydrogenation

Yangzhi Xu,Zirui Gao,Yao Xu,Xuetao Qin,Xin Tang,Zhiwei Xie,Jinrong Zhang,Chuqiao Song,Siyu Yao,Wu Zhou,Ding Ma,Lili Lin

Hydrogenation of CO 2 into methanol at low-temperature on Cu-based catalysts is of great significance, but remains challenging to enhance activity. In this paper, we report an inverse catalyst constructed with nano-ZrZnO x supported on Cu particles with outstanding methanol synthesis performance at 220 ℃, two times higher than that of commercial Cu/ZnO/Al 2 O 3 catalysts under the same conditions. Detailed structure characterization and performance evaluation demonstrate that the ZrZnO x mixed oxide serves as the most active oxide-metal interface site for CO 2 hydrogenation. The ZrZnO x /Cu inverse catalyst increases the weak and medium CO 2 adsorption sites which are further demonstrated responsible to the methanol productivity. In situ DRIFTs studies reveal that the inverse interface accelerates the reduction of asymmetric formate intermediates and prevents the generation of CO. The combination of enhanced CO 2 activation capability and accelerated hydrogenation rate of intermediates over the ZrZnO x /Cu inverse catalyst probably contribute to the remarkable methanol synthesis performance from CO 2 .

CAS / MDL: 144-62-7
研究领域: 催化化学 · 能源化学 · 材料科学
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