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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH · 2023 ·Vol. 30 ·期 42 ·95425-95437 · IF 5.8

Degradation performance of methylene blue in metal nanoparticle modified 3D mesoporous wood microchannels

Zheng Guanfeng,Fu Peng,Li Zhiyu,Zhang Yuchun,Huang Xinfeng,Chen Jieming

Wood has a rich three-dimensional pore structure and many bottom-up nanochannels. However, the structure of wood itself has limited ability to adsorb dyes, so the effective combination of the unique structure of wood and Pd NPs was studied to achieve efficient degradation of dyes. First, the three-dimensional structure of natural wood is optimized by combining the complex pore structure of wood with Pd NPs to improve the contact process between the dye and Pd NPs. Then, Pd (II) ion can be well reduced to Pd NPs by wood lignin. In addition, Pd NPs can be fixed by hydroxyl groups on cellulose in wood. The flow state inside Pd NPs/wood film and the contact area between catalyst and dye were discussed in detail by hydrodynamic simulation, which filled the gap. It provides reference for composite structure. When Pd NPs/wood membrane was used to treat methylene blue (MB), the degradation efficiency was up to 96.7%, which was 90% higher than that of natural wood. Its TOF value was 1.82 mol MB  mol Pd −1 min −1 , which was higher than that in the previous literature. Therefore, the novelty of this study is that the mechanism of catalytic degradation of MB by Pd nanoparticles/wood composites is reported for the first time. The internal flow mode and contact condition of the new material are understood, which has a good application prospect. Graphical Abstract

研究领域: 环境科学 · 材料科学 · 化学工程
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2020 · IF 4.939

Mo-doped Ni-based catalyst for remarkably enhancing catalytic hydrogen evolution of hydrogen-storage materials

Yutong Wang,Lun Pan,Yixin Chen,Guoqiang Shen,Li Wang,Xiangwen Zhang,Ji-Jun Zou

Ni-based alloys are considered as the efficient catalyst for hydrogen-storage materials decomposition. Herein, we applied an in-situ melt-quenching method to dope Mo in Ni-based alloy for catalytic hydrogen evolution from hydrogen-storage materials. Importantly, Mo doped Ni-based catalyst exhibits more than 6 times higher TOF value than that of pure Ni both in AB hydrolysis and hydrazine decomposition, because Mo acts as an electron donor to improve the reducibility of Ni. Hydrogen evolution kinetics were studied over a range of temperatures (303–353 K) and initial feed concentrations (catalyst/hydrogen-storage materials (wt/wt) ratios = 0.2–10). Under optimal reaction conditions, the H 2 evolution rate reaches 1.92 mol H 2 /(mol cat  min) and 0.05 mol H 2 /(mol cat  min) in the hydrolysis of ammonia borane and decomposition of hydrazine, which are 6.42 and 6.44 times higher than undoped Ni catalyst, respectively. And the apparent activation energy of ammonia borane hydrolysis and hydrazine decomposition were evaluated to be 26.66 ± 3.31 kJ/mol and 40.01 ± 3.38 kJ/mol, respectively.

CAS / MDL: 13774-81-7
研究领域: 材料科学 · 催化化学
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2022 · IF 7.139

Nitrogen-phosphorus co-functionalized reduced graphene oxide supported NiCoPd-CeOx nanoparticles as a highly efficient and stable catalyst for formic acid dehydrogenation

Jia-Yun Wang,He-Nan Shang,Di Liu,Si-Jia Li,Ya-Xuan Bai,Yu-Bo Liu,Jin-Sheng Liang

Formic acid (HCOOH, FA), a common liquid hydrogen storage material, has attracted tremendous research interest. However, the development of efficient, low-cost and high-stable heterogeneous catalyst for selective dehydrogenation of FA remains a major challenge. In this paper, a simple co-reduction method is proposed to synthesize nitrogen-phosphorus co-functionalized rGO (NPG) supported ultrafine NiCoPd-CeO x nanoparticles (NPs) with a mean size of 1.2 nm. Remarkably, the as-prepared Ni 0.2 Co 0.2 Pd 0.6 -CeO x /NPG shows outstanding catalytic activity for FA dehydrogenation, affording a high TOF value of 6506.8 mol H 2 mol Pd −1 h −1 at 303 K and a low activation energy of 17.7 kJ mol −1 , which is better than most of the reported heterogeneous catalysts, and can be ascribed to the combined effect of well-dispersed ultrafine NiCoPd-CeO x NPs, modified Pd electronic structure, and abundant active sites. The reaction mechanism of dehydrogenation of FA is also discussed. Furthermore, the optimized Ni 0.2 Co 0.2 Pd 0.6 -CeO x /NPG shows excellent stability over 10 th run with 100% conversion and 100% H 2 selectivity, which may provide more possibilities for practical application of FA system on fuel cells.

研究领域: 催化 · 材料科学 · 能源存储 · 纳米技术
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CATALYSIS LETTERS · 2021 ·Vol. 152 ·期 7 ·2164-2177 · IF 3.186

Highly Effective Rh/NaNbO3 Catalyst for the Selective Hydrogenation of Benzoic Acid to Cyclohexane Carboxylic Acid Under Mild Conditions

Hu Yin,Chen Wei,Chen Yongxin,Zhang Fen,Song Weiguo,Wang Lingling,Fu Jianping,Ren Xiangrong,You Shengyong,Cao Changyan,Yu Zhonghua,Dong Xiaona

Rh/NaNbO 3 catalyst was prepared by a facile solvothermal method combined with photo-deposition technique. Over this catalyst, both conversion and selectivity were up to 100.0% in ten reaction recycles for the selective hydrogenation of benzoic acid to cyclohexane carboxylic acid at room temperature and 0.5 MPa H 2 pressure. TOF value of the catalyst was 207 h −1 for this hydrogenation reaction. The excellent performance and the mild hydrogenation conditions were among the best of the reference catalysts with different supports or surface metal active component. Multiple characterization techniques were adopted to further study the essence of the superior hydrogenation performance. It was found that the abundant oxygen vacancies and the reduction in situ of Rh species accounted for the excellent hydrogenation performance. Besides, the reducible perovskite support, small Rh species particle, specific morphology and pore structure of the catalyst also played important roles in improving the hydrogenation reaction. After eleven hydrogenation recycles, the inactivation of the catalyst was also investigated, and attributed to the carbon deposition and the leaching of Rh species during hydrogenation process. It is an attractive work to design the highly efficient catalysts for benzoic acid hydrogenation with potential application value. Graphic Abstract

研究领域: 催化 · 化学工程 · 材料科学
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GREEN CHEMISTRY · 2022 ·Vol. 24 ·期 18 ·6945-6954 · IF 11.034

Targeted regulation of the selectivity of cascade synthesis towards imines/secondary amines by carbon-coated Co-based catalysts

Songtao Huang,Zijiang Zhao,Zhongzhe Wei,Mingxuan Wang,Yi Chen,Xiaosa Wang,Fangjun Shao,Xing Zhong,Xiaonian Li,Jianguo Wang

Imines and secondary amines have attracted widespread attention in the fields of medicine owing to their unique unit structures and biological activities. However, the design of catalysts for the targeted syntheses of imines and secondary amines presents challenges due to the uncontrollable cascade reaction of nitrobenzene (NB) and benzaldehyde (BA). Herein, we report that carbon-coated Co and PtCo catalysts (Co/SiO2@CN and PtCo/SiO2@CN) realize the directional synthesis of imines and secondary amines under the same conditions, respectively, through the synergistic action of the active components. The superior catalytic performance benefited from the integrated geometric and electronic effects. Specifically, the uniformly coated nitrogen-doped carbon drives the adsorption ability of NB more strongly than BA and inhibits the formation of benzyl alcohol. For Co/SiO2@CN, Co–Nx and metallic Co synergistically promote the highly selective synthesis of imines with much higher conversion (97%) and selectivity (98%) than most Co-based catalysts at 60 °C. For PtCo/SiO2@CN, the electron transfer between Pt and Co promotes the hydrogen spillover ability and enables it to afford 100% BA conversion and 100% secondary amine selectivity, reaching the TOF value of 296 h−1. This synthesis strategy provides an advanced concept for designing chemoselective catalysts, which has important implications for both scientific research and industrial applications.

研究领域: 催化 · 有机化学 · 材料科学 · 药物化学
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RENEWABLE ENERGY · 2020 · IF 6.274

Monodispersed bimetallic nanoparticles anchored on TiO2-decorated titanium carbide MXene for efficient hydrogen production from hydrazine in aqueous solution

Feng Guo,Hongtao Zou,Qilu Yao,Bin Huang,Zhang-Hui Lu

Selective catalytic decomposition of hydrazine (N 2 H 4 ) to provide a clean energy carrier hydrogen (H 2 ) is a promising alternative to fossil fuels for the future energy economy. NiPt nanoparticles (NPs) dispersed on delamination of TiO 2 -decorated Ti 3 C 2 T x (denoted as DT-Ti 3 C 2 T x ) nanosheets are prepared via a simple wet chemical reduction method and applied as an efficient catalyst for dehydrogenation of N 2 H 4 in aqueous solution. The rich oxygen-containing functional groups on the surface of DT-Ti 3 C 2 T x not only facilitate the formation and immobilization of monodisperse NiPt NPs but also enhance the synergistic effect between metal NPs and MXene support. Among all of the tested samples, the optimized Ni 0.8 Pt 0.2 /DT-Ti 3 C 2 T x nanocatalyst exhibits the 100% H 2 selectivity and best catalytic performance with a TOF value of 1220 h −1 for the selective decomposition of N 2 H 4 at 323 K. In addition, this catalyst also shows excellent catalytic performance for hydrogen production from hydrazine borane (N 2 H 4 BH 3 ) via the hydrolysis of borane group and selective decomposition of hydrazine moiety. The TiO 2 -decorated Ti 3 C 2 T x MXene can be applied as an excellent support to obtain well-dispersed and ultrafine metal NPs for various applications.

研究领域: 材料科学 · 催化 · 能源存储与转换 · 纳米技术
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