INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2023
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IF 7.2
Minglei Lu,Shuting Liu,Haiping Zhu,Haifeng Huang,Chunying Lin,Jianxian Li,Baofang Zhang,Zefeng Zheng,Changsong Hu,Xiaoping Wu,Geli Liu,Tiejun Wang
Highly efficient releasing of hydrogen by aqueous-phase reforming of methanol (APRM) is of great significance to promote the development of stationary and mobile H 2 power supply for polymer electrolyte membrane fuel cells (PEMFCs). However, highly active catalysts with excellent performance of in situ releasing H 2 from APRM still face challenges. Herein, we report a Cu-SP/Al 2 O 3 –ZnO (Cu-SP/AZ) catalyst prepared by carbon layer encapsulated hierarchical porous microsphere strategy, which enhanced Cu dispersion (52.8 wt% loading, ∼5 nm particle size) on Al 2 O 3 –ZnO (AZ) microsphere . The proposed catalyst exhibited high H 2 production rate (base-free) of 64.23 μmolH 2 /gcat/s at 210 °C, which was nearly the same as that of 20% Pt/C catalyst (63.86 μmolH 2 /gcat/s) and 2.6-fold higher than that of commercial CuO/ZnO/Al 2 O 3 catalyst (24.62 μmolH 2 /gcat/s). The characterization results demonstrated that its high activity in APRM could be ascribed to the strategy of carbon layer encapsulated hierarchical porous microsphere as well as coordination of hydroxyl functional group of SP with Cu 2+ .
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高影响因子
JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
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2019
·
IF 4.029
Jie Zhang,Xiangcheng Li,Wei Gong,Pingan Chen,Boquan Zhu
Columnar β-Sialon bonding phases were in situ synthesised in Al 2 O 3 -C refractory composites and their growth mechanism was simulated based on first-principles calculations. The experimental results indicated that the addition of Fe 2 O 3 as a catalyst accelerated the transformation of Si 3 N 4 to β-Sialon, resulting in a well-developed columnar structure. The (100) facet was the primary surface for crystal growth during the transformation process of Si 3 N 4 into β-Sialon. According to first-principles calculations, the surface energy of the (100) facet decreased greatly due to the substitution of (Si, N) pairs with (Al, O). The catalyst could promote the adsorption of gaseous phases on the (100) facet of Si 3 N 4 and decreased the gas adsorption energy of both SiO and Al 2 O. Owing to the presence of in situ synthesised columnar β-Sialon bonding phases, the residual crushing strength of Al 2 O 3 -C refractory composites after 5 thermal shock cycles increased by 25.1%.
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Surfaces and Interfaces
·
2024
·
IF 5.7
Xiangming Yang,Yan Liu,Yuting Zhong,Hui Chen
Superhydrophobic coatings simultaneously exhibiting high substrate binding, mechanical durability and self-healing properties are of great significance for anti/de-icing applications. In this study, we fabricated a high substrate binding and mechanical durability anti/de-icing superhydrophobic coatings (SL-AP/SPS-SiO 2 ) with self-healing performance by spray-coating a photothermal self-healing organic layers (AP/SPS-SiO 2 ) plasma-sprayed porous Al 2 O 3 –13%TiO 2 underlayer (SL), the resulting soft-hard interlocking structure significantly increased the adhesion strength of the coating to 16.7 ± 0.36 MPa while reducing the ice adhesion strength to 46.5 ± 3.0 kPa. In the as-obtained organic layers, self-stratifying acrylic resin (AR)/20%polymethylsiloxane (PDMS) (AP), not only enhanced the bonding strength with the underlayer but also imparted photothermal self-healing capability to the coating through the action of the photothermal agent (SPS-SiO 2 ). And sodium alginate (SA) guided the self-oxidative polymerization of dopamine (DA) and its deposition on hydrophilic SiO 2 to form a π-π stacked fiber structure photothermal agent (SPS), after hydrophobic SiO 2 modification increased the coating's roughness and photothermal performance. Remarkably, the coating achieved a contact angle of up to 158.4 ± 0.89° and a rolling angle of 3.5 ± 0.89°, maintaining its superhydrophobic properties even after exposure to acid-base immersion and mechanical abrasion. Furthermore, the coating exhibited self-healing capabilities in superhydrophobicity against O 2 plasma etching, with a contact angle recovery rate of up to 98.9% after undergoing 10 cycles of O 2 plasma etching and light exposure. Enhancing mechanical and chemical stability with self-healing capabilities is beneficial for extending the lifespan of superhydrophobic coatings used in anti-/de-icing applications.
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Surfaces and Interfaces
·
2024
·
IF 5.7
Chengzhi Wang,Zhenbang Tian,Weiqing Huang,Jingyuan Hu,Xing Xing
Owing to the different reaction properties and deactivation mechanisms caused by the structural discrepancy of monolithic catalysts, abundant scientific results of powder or granular NH 3 -SCR catalysts have still not sufficiently robustly applied in recent years. Furthermore, minimal research has been focused on monolithic catalysts. As a result, this work prepared monolithic Mn-Fe-Ce/Al 2 O 3 catalysts by active component impregnation (ACI-Mn-Fe-Ce/Al 2 O 3 ) and precursor impregnation methods (PI-Mn-Fe-Ce/Al 2 O 3 ) and investigates the long-term SO 2 and H 2 O resistance of the catalysts. Compared with the PI-Mn-Fe-Ce/Al 2 O 3 catalyst, the monolithic ACI-Mn-Fe-Ce/Al 2 O 3 catalyst showed better performance. The catalytic activity follows a bell-shaped curve with an optimal performance at a drug loading of 5 %. The ACI-Mn-Fe-Ce/Al 2 O 3 catalyst exhibits long-term resistance to SO 2 and H 2 O and can still convert more than 70 % NO x after 168 h of SO 2 and H 2 O resistance test. Characterization of the ACI-Mn-Fe-Ce/Al 2 O 3 catalysts before and after the reaction showed that the reducibility decreased after the reaction, and more Mn 4+ was transformed into Mn 2+ to weaken the catalytic activity. However, more Fe 2+ and Ce 3+ were generated during the reaction, increasing the number of oxygen vacancies, oxygen defects, and hydroxyl-like groups, all of which would contribute to a certain extent to counteract the passivation effect of SO 2 on the catalysts. In situ DRIFTs analysis shows that the formation of surface sulfates has a minimal effect on the adsorption of NO, but it does affect the adsorption of coordinated NH 3 on Lewis acid sites. This work elucidates the deactivation details of Mn-Fe-Ce/Al 2 O 3 catalysts from the perspective of physicochemical properties, which provides a reference for the development of better low-temperature SO 2 -resistance catalysts for industrial applications.
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JOURNAL OF HAZARDOUS MATERIALS
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2025
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IF 11.3
Qiuyu Chen,Yongyi Zhang,Haiwang Liu,Peng Liu,Xinxin Ye,Xing Xia,Xiangwei Wu
Straw-derived dissolved organic matter (DOM) is widespread in farmland soils, but the relationship between straw-derived DOM and As in their co-sorption on minerals and the underlying mechanisms remain unclear. Here, batch experiments and spectroscopic analyses were employed to investigate the co-sorption of straw-derived DOM and As(III/V) on γ-Al 2 O 3 . Results showed a trade-off between the As(III/V) and DOM immobilization on γ-Al 2 O 3 under different pH levels, which was caused by competitive sorption. The rape straw-derived DOM (DOM_Ra) exhibited a stronger inhibition on As(III/V) sorption than rice straw-derived DOM (DOM_Ri). This could be due to more aromatic fractions in the DOM_Ra and DOM_Ri, which were preferentially sorbed by γ-Al 2 O 3 . In turn, the preferential sorption of aromatic DOM components was weakened by As(V) sorption, which, however, was not found in As(III) and DOM co-sorption. Furthermore, spectral results indicated that carboxylic groups on the sorbed DOM could provide additional binding sites for As(III/V) to form ternary complexes, but its role was overwhelmed by the DOM competitive sorption, which ultimately exhibited the inhibitory effect of DOM on As(III/V) sorption. These findings enhance the fundamental understanding of the co-sorption of As(III/V) and DOM on soil minerals and contribute to predicting As mobility and OM stability in As-contaminated farmlands with straw return.
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PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2021
·
IF 5.816
Xiang Gong,Shuyi Guo,Zhao Jiang,Bolun Yang,Tao Fang
Hydrogen is a promising candidate to substitute the fossil fuels. However, the efficient hydrogen storage technologies restrict the commercial applications. Developing new catalysts with high activity and selectivity is important for the dehydrogenation reaction in N-ethylcarbazole/dodecahydro-N-ethylcarbazole (NECZ/12H-NECZ) hydrogen storage system. In this work, a series of Pd-M/Al 2 O 3 (M = Co, Ni and Cu) bimetallic catalysts are synthesized successfully and show good performance in the dehydrogenation reaction of 12H-NECZ than the commercial Pd/Al 2 O 3 catalyst. The Pd 1 Co 1 /Al 2 O 3 catalyst (Practical Pd content = 2.4136 wt%) showed the highest catalytic performance with 95.34% H 2 release amount, TOF of 230.5 min −1 and 85.4% selectivity of NECZ. Combined with the characterization analysis, it can be proposed that the dehydrogenation performance of 12H-NECZ is dependent on the alloy phases , reasonable electronic structures and nanoparticle size of catalysts. The fine-tuned alloy degree and appropriate nanoparticle size of Pd 1 Co 1 /Al 2 O 3 bring the 17.7% increase of H 2 release amount and 99.5% increase of NECZ selectivity than those of Pd/Al 2 O 3 . For the bimetallic catalysts, the enhancement of selectivity of NECZ is mainly from the increase of the kinetic constant of rate-limiting step.
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Catalysis Science & Technology
·
2019
·Vol. 9
·期 21
·6037-6046
·
IF 5.726
Min Zhong,Jungang Wang,Congbiao Chen,Zhancheng Ma,Litao Jia,Bo Hou,Debao Li
Herein, the shell–core-structured SiC–Al2O3@Al composite consisting of an Al metal core and a SiC–Al2O3 hybrid shell was synthesized by a straightforward preparation method. Compared with Al2O3@Al composites, the SiC-modified samples possess a meso–macroporous structure, high pore volume, wide pore size, and a special surface where active and inert components coexist. The ratio of inert to active components on the composite surface could be modulated by controlling the amount of SiC nanoparticles (NPs). Upon the decoration of SiC NPs, the degree of reduction of cobalt oxides and the density of active sites (Co0) increased significantly. Moreover, the SiC-modified catalysts exhibited lower apparent activation energy (Ea) and higher intrinsic reaction rate (TOF) mainly due to the electron-rich properties of Co NPs in the modified samples. Accordingly, the cobalt-weight normalized FT activity (CTY) of the SiC-modified catalysts increased by a factor of about 1.6–2.0. Moreover, the catalyst modified by the SiC NPs showed lower selectivity towards light hydrocarbons (CH4 and C2–C4) but higher selectivity towards long-chain hydrocarbons (C5+). When the mSiC/mAl ratio was 15%, the CoAC-15 catalyst showed maximum density of active sites and highest TOF, leading to highest activity and C5+ selectivity (approximately 92%). The synergistic effect of the SiC–Al2O3 hybrid shell and the Al metal core was beneficial for the catalytic properties of the Co/SiC–Al2O3@Al catalysts. The binary SiC–Al2O3 nanostructure endowed the Co NPs with electron-rich characteristics to enhance the CO activation; moreover, the special surface where the active and inert components coexisted improved the reducibility of cobalt oxides, and the abundant porosity of the hybrid shell facilitated the transfer of reactants and products. In addition, the existence of the Al metal core improved heat transfer in the reaction.
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ACS Sustainable Chemistry & Engineering
·
2026
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IF 7.3
Wenjun Zhang,Zijiang Zhao,Yonggang Gang,Xiaosong An,Liboting Gao,Siyi Bao,Xuping Ren,Jun Wang,Jianhua Yan,Hao Zhang
Cu/ZnO/Al2O3 (CZA) catalyst remains the benchmark for methanol synthesis but suffers from active-site sintering and insufficient CO2 activation. In this study, we proposed a dual strategy to enhance and regulate the active sites of CZA: hydrothermal treatment induces Cu–Zn coordination to create high-density Cu–ZnO1–x interfaces that promote CO2 conversion, while subsequent La doping regulates Cu0/Cu+ species to favor methanol selectivity. As a result, the maximum space-time yield (STY) of methanol over the designed CZA&5%La-LRCP (prepared by the ligand-regulated coprecipitation method) catalyst improved significantly from 283.0 gMeOH·kgcat–1·h–1 for the conventional coprecipitation-prepared CZA to 400.4 gMeOH·kgcat–1·h–1 under the tested conditions, surpassing most literature reports on La-doped Cu-based catalysts. Comprehensive characterizations and kinetic studies revealed that high-density Cu–ZnO1–x interfaces enhance CO2 adsorption and activation, while uniformly distributed electron-enriched Cu0/Cu+ species promote H2 dissociation and facilitate formate formation and transformation, together establishing an efficient pathway for CO2 activation and hydrogenation. This study demonstrates a promising strategy for the rational design of CO2hydrogenation catalysts through the synergistic modulation of interfacial structure and electronic properties.
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高影响因子
ACS Sustainable Chemistry & Engineering
·
2026
·
IF 7.6
Liu Mengyu,Feng Wenji,Wu Yunshuo,Wang Haiqiang,Wu Zhongbiao
Methane valorization is important for climate change mitigation and sustainable carbon utilization, but conventional nonoxidative coupling of methane (NOCM) suffers from the high activation barrier of CH 4 , limited product selectivity, and rapid coking-induced deactivation. Herein, we develop a spark discharge−dielectric barrier discharge (DBD) coupled plasma-catalytic system for the selective conversion of high-concentration methane to ethylene. Spark discharge first activates CH 4 and preferentially converts it to C 2 H 2 , while a downstream catalyst bed, maintained at 100−130 ° C by residual discharge heat, enables acetylene semihydrogenation to C 2 H 4 . A coupled DBD unit is further introduced for in situ carbon removal and catalyst regeneration. Among the tested catalysts, impregnation−reduction-derived 0.1Pd-5Cu/γ-Al 2 O 3 -R with atomically dispersed Pd exhibited the best performance, achieving 72.38% CH 4 conversion, 72.19% C 2 H 4 selectivity, 92.48% acetylene-based C 2 H 4 selectivity, and a C 2 H 4 space-time yield of 69.97 mmol·g· −1 ·h −1 at 36.2 kJ·L −1 . With DBD-assisted regeneration, efficient NOCM operation was maintained for 630 min. Mechanistic analyses associate the enhanced ethylene selectivity with highly dispersed Pd sites and their electronic modulation by predominantly low-valent Cu species, which suppress overhydrogenation and facilitate ethylene desorption.
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高影响因子
WATER SCIENCE AND TECHNOLOGY
·
2020
·Vol. 83
·期 2
·257-270
·
IF 1.638
Qu Guangzhou,Wang Hui,Li Xin,Wang Tiecheng,Zhang Zengqiang,Liang Dongli,Qiang Hong
This paper presents a study of V and N co-doping TiO 2 embedding multi-walled carbon nanotubes (MWCNTs) supported on γ -Al 2 O 3 pellet (V/N-TiO 2 -MWCNTs/ γ -Al 2 O 3 ) composite photocatalyst induced by pulsed discharge plasma to enhance the removal of acid orange II (AO7) from aqueous solution. The photocatalytic activity of the V/N-TiO 2 -MWCNTs/ γ -Al 2 O 3 composite to AO7 removal induced by the pulsed discharge plasma was evaluated. The results indicate that the V/N-TiO 2 -MWCNTs/ γ -Al 2 O 3 composite possesses enhanced photocatalytic activity that facilitates the removal of AO7 compared with the TiO 2 -MWCNTs/ γ -Al 2 O 3 and TiO 2 / γ -Al 2 O 3 composites. Almost 100% of AO7 is removed after 10 min under optimal conditions. The V 0.10 /N 0.05 -TiO 2 -MWCNTs/ γ -Al 2 O 3 photocatalyst exhibits the best removal effect for AO7. Analysis of the removal mechanism indicates that the enhancement of the removal of AO7 resulting from V and N co-doping causes TiO 2 lattice distortion and introduces a new impurity energy level, which not only reduces the band gap of TiO 2 but also inhibits the recombination of the pairs. An efficient and easily recycled V/N-MWCNTs-TiO 2 / γ-Al 2 O 3 composite was prepared. Activity of the composite induced by discharge plasma to AO7 removal was evaluated. Synergistic effect of discharge plasma and catalyst effectively improve AO7 removal. The composite demonstrates adequate recycling performance in a discharge plasma system. Possible mechanisms of AO7 removal were analyzed.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Chen Chang,Xin Guan,Panpan Wang,Xingping Zhou,Xiaolin Xie,Yunsheng Ye
The development of lithium-sulfur (Li-S) batteries is dogged not only by severe limitations in cycling and rate performances arising from the shuttle effect of lithium polysulfides (LiPSs) but also severe degradation under harsh evaluation conditions of high sulfur loading, lean-electrolyte, and prominent thermal gradient . To achieve high performance and safety in Li-S batteries, a flexible and multifunctional integrated interlayer consisting of dual-functional alumina/carbon (Al 2 O 3 /C) nanofiber skeleton and organosilicon (OSi) filler is fabricated. Electrically and thermally conductive nanofibers are continuous and interlaced, enhancing the reutilization of LiPSs and the homogenization of temperature gradient through constructed dual-conductive networks. The interval-filled OSi helps in the diffusion of LiPSs and the absorption and retention of electrolytes, providing significant support to stabilize the Li-S batteries for long-term cycling. As a result, considerable enhancements in cycle stability and rate performance either under a high sulfur loading of ∼5.5 mg cm - 2 , low electrolyte/sulfur (E/S) rate of 4 μL mg - 1 , or artificial temperature gradients are achieved for a typical sulfur/carbon black cathode simply by incorporating multifunctional Al 2 O 3 /C@OSi interlayer. The new design and configuration of the interlayer may practically be used in high-energy applications since it can effectively address severe limitations of the current Li-S batteries.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Rosine Ahishakiye,Fumin Wang,Xubin Zhang,Mingshuai Sun,Yi Zhai,Yongkui Liu,Yuzhou Wu,Mengyue Li,Mengyao Li,Qing Zhang
The efficient production of the liquid fuel 2,5-dimethylfuran (DMF) from biomass-derived 5-hydroxymethylfurfural (HMF) is very complicated because of the presence of the aldehyde group, hydroxyl group, and C C bond. In this study, a novel Co-CoOx –FeNiCo/γ-Al 2 O 3 catalyst was developed for selective hydrogenation of HMF to DMF. The catalyst was characterized by using XRD, TEM , SAED , BET, XPS, NH 3 -TPD, and H 2 -TPR techniques. The catalyst reduced at 500 °C exhibited excellent catalytic performance and the highest DMF yield (>99.9%) was obtained at 190 °C and 4 h. During the reaction, metal sites selectively hydrogenated the C O bond while acid sites (CoOx acid sites) selectively hydrogenolyzed C O bond. Appropriate surface acidity of the catalyst and the balance between metal and metal oxide species are the main factors for achieving a high yield of DMF. At reaction temperatures below 150 °C, DMF was not produced and HMF has completely converted into 2,5-Bis(hydroxymethyl)furan (BHMF), an important furan diol for polymers production. 100% BHMF yield was also obtained for the HMF hydrogenation over 300 °C reduced catalysts due to the high concentration of strong acid sites. The catalyst recyclability exhibited excellent stability and the original activity was maintained after six reuses. A reaction mechanism was also proposed.
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高影响因子
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