JOURNAL OF CATALYSIS
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2017
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IF 6.844
Lingfeng Shen,Shanjun Mao,Jianqing Li,Mingming Li,Ping Chen,Haoran Li,Zhirong Chen,Yong Wang
This work highlights a novel hybrid catalyst, intermetallic PdZn on CN@ZnO (PdZn/CN@ZnO), which serves as a highly efficient heterogeneous catalyst for semihydrogenation of 2-methyl-3-butyn-2-ol utilizing water as the solvent. Compared with intermetallic PdZn on ZnO (PdZn/ZnO), PdZn/CN@ZnO displays almost sixfold higher TOF while retaining high selectivity. It is assumed that the introduction of biomass-derived hydrophilic nitrogen-doped carbon into the ZnO helped to promote catalyst dispersion in aqueous media, ensuring better mass transfer. Further experiments and theoretical calculations showed that from Pd particles to intermetallic PdZn, the decrease of corner and edge Pd atoms might be a factor leading to the improvement of selectivity. Recycling experiments demonstrated that the PdZn/CN@ZnO catalyst could be reused at least eight times without significant decrease in activity or selectivity. Furthermore, when applied to industrially relevant alkenols that are building molecules for the production of vitamin E, the present catalyst still offered excellent performance. It is expected that the present catalytic system will demonstrate its high potential for practical production of vitamin E.
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FUEL
·
2017
·
IF 4.601
Sainan Wei,Huijun He,Yan Cheng,Chunping Yang,Guangming Zeng,Li Kang,Hui Qian,Canyao Zhu
Sulfur-containing compounds in oils are harmful to the ecosystem whose cost-effective removal is still a challenge. In this study, novel heterogeneous catalysts of cobalt supported on KIT-6 mesoporous silicas were prepared and evaluated for oxidative desulfurization (ODS) under ambient conditions using cyclohexanone peroxide (CYHPO) as the oxidant. The model oil was obtained via dissolving DBT in the n-octane. The conventional wet impregnation method was applied for the preparation of the catalysts, and cobalt nitrate was used as the precursor. The catalysts were characterized by XRD, N 2 -physisorption, FT-IR, TGA, SEM/TEM and XPS. Then their catalytic activities in total oxidation of dibenzothiophene (DBT) were evaluated at various conditions. DBT conversion by this heterogeneous ODS system reached 98.68%. Co/KIT-6 catalysts showed high ODS activity due to Ia3d mesoporous structure resulting in better cobalt dispersion, higher activity of Co, and faster diffusion of reactant and products. The Box-Behnken design showed that the optimum values for the conversion of DBT were 93 °C (oxidation temperature), 1.6 × 10 −1 g (catalyst amount) and 5.7 (O/S molar ratio), respectively. The inhibitory effect of quinoline on ODS was higher than carbazole and indole, adding quinoline into model oil under same conditions led to a decrease of the conversion of DBT from 98.68% to 65.67% when the concentration of quinoline increased from 160 ppm to 4845 ppm. Kinetics data correlated well with the pseudo-first-order equation. These data showed that this novel Co/KIT-6 catalysis system has the potential to be applied in ODS from oils.
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GREEN CHEMISTRY
·
2016
·Vol. 18
·期 22
·6082-6090
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IF 8.506
Minghui Tang,Jiang Deng,Mingming Li,Xuefeng Li,Haoran Li,Zhirong Chen,Yong Wang
Ruthenium nanoparticles (2.6 nm) uniformly dispersed on a three-dimensional (3D) interconnected hierarchical porous N-doped carbon (Ru/NHPC) have been successfully developed, serving as a highly active and stable catalyst for the selective hydrogenation of aromatics under mild conditions. A novel “leavening” strategy, i.e. using biomass-derived α-cellulose as a carbon precursor and ammonium oxalate as both a nitrogen source and foaming agent, affords the NHPC material a large surface area (870 m2 g−1), an excellent hierarchical nanostructure which acts as a convenient mass transfer channel and a high ability in stabilizing and dispersing Ru nanoparticles. The Ru/NHPC catalyst exhibits a substantially enhanced activity for the hydrogenation of toluene (TOF up to 39 000 h−1) and quinoline (TOF up to 2858 h−1) in comparison with Ru/HPC (3D-hierarchical porous carbon without nitrogen doping) and Ru/AC (commercial activated carbon) under the same reaction conditions. Further investigations indicate that the 3D interconnected porous structure and N-doping contribute to the improved diffusion and mass transfer, homogeneous dispersion of ruthenium nanoparticles and high percentage of Ru0 (active sites), which results in considerable catalytic performance. This work offers great potential for the application of supported catalysts based on NHPC materials in fine chemical production with high activity.
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DYES AND PIGMENTS
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2016
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IF 4.055
Hailong Wang,Lele Zhao,Xueqiang Liu,Jing Xu,Wenlong Hou,Jianmin Wang,Enfang He,Ruijun Zhang,Haiquan Zhang
Among photocatalytic materials, p-n heterojunction-type photocatalysts has good photocatalytic performance under visible light irradiation. Herein, a novel Copper phthalocyanine/perylene diimide derivatives p-n heterojunction photoeatalysts based on the intermolecular hydrogen bond between pyridyl and carboxyl was designed and characterized using FT-IR, UV–vis and photoluminescence spectra, and then compared their photocatalytic performance by degradation for rhodamine B (RhB) under visible light irradiation. The hydrogen bond composites shows significant higher photocatalytic activity comparing with its parent, and the photocatalysis increased with increasing of mole fraction of perylene diimide derivatives. The change of morphology and p-n heterojunction structure are in favor of the high photocatalytic active. Furthermore, the photocatalytic mechanism was investigated by radical scavengers testing, that confirmed hydroxyl radical ( OH) was the main reactive species for the degradation of RhB.
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FUEL
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2017
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IF 4.601
Youan Ji,Yucui Hou,Shuhang Ren,Muge Niu,Congfei Yao,Weize Wu
Indole plays a significant role in the production of products such as spices, medicines, and exogenous auxins. Deep eutectic solvents (DESs) formed by indole and quaternary ammonium salts (QASs, including tetraethylammonium chloride-TEAC, tetrapropylammonium chloride-TPAC, triethylmethyl-ammonium chloride-TEMAC) were found and proposed to efficiently extract indole from model wash oil. The effects of time, temperature, mole ratio of QAS to indole and initial indole concentration on the extraction of indole were studied. The results indicate that these QASs can extract indole from wash oil with efficiencies up to 96.7% (TPAC). The extraction process can be finished within 5 min. It is also found that the ultimate concentrations are almost identical for one kind of QAS although their initial concentrations are different, and the indole concentration in model wash oil can be reduced to a very low level of 1.3 g/dm 3 (TPAC). The maximum distribution coefficients of indole are 40.8 for TEAC, 91.9 for TPAC, and 29.5 for TEMAC at the studied conditions, and the extraction ability follows the order of TPAC > TEAC > TEMAC. Moreover, QASs in DESs can be reused without obvious reduction in extraction efficiency. The extraction mechanism was studied by FT-IR, and the results indicate that there is a hydrogen bond between QAS and indole. Finally, a comparison was made between this method and other methods to verify and demonstrate its desirable properties of efficiency and environmentally friendliness.
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Small
·
2025
·
IF 12.1
Zhefei Zhao,Wenjie Yan,Wenbin Zheng,Lipeng Guo,Ruopeng Yu,Minhao Chen,Huajun Zheng
Electrocatalytic hydrogenation (ECH) of quinoline provides an eco-friendly and prospective route to achieve the highly value-added generation of 1,2,3,4-tetrahydroquinoline (THQ). Co element has been proven to be the efficient catalytic site for ECH of quinoline, but the rational regulation of the electronic structure of active Co site to improve the activity is still a challenge. Herein, the hierarchical core–shell structure consisting of NiCo-MOF nanosheets encapsulated Cu(OH) 2 nanorods (Cu(OH) 2 @CoNi-MOF) is constructed. The heterojunction promotes the transfer of interfacial charge and optimizes the electronic structure of the Co site. The introduction of Ni significantly increases the binding between Co and Cu, preventing the exfoliation of Co sites from Cu(OH) 2 core, and reducing the reaction energy barrier of rate-determining step, thus resulting in superior reactivity and durability. Besides, electrochemical reconstruction further modulates the electronic structure of Co by forming the multi-metallic compound with a low valence state (NiCoCu), achieving an optimal performance with a conversion of 99.5% and THQ selectivity of 100%. A flow-cell system is assembled, demonstrating the prospect for industrial application.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2025
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IF 8.3
Zhenye Zhang,Shenghan Zhang,Shijie Wang,Xinliang Guo,Zhilin Wang,Yu Tan,KeXin Liang
Liquid organic hydrogen carriers (LOHCs) are considered highly promising materials for hydrogen storage due to their potential to store hydrogen under mild conditions. However, traditional hydrogenation and dehydrogenation methods for LOHCs often require harsh conditions and rely on exogenous hydrogen donors, limiting their practical application. Therefore, developing an efficient method to catalyze LOHCs hydrogenation and dehydrogenation at room temperature using a safe and clean hydrogen source is of significant scientific and practical importance. This paper presents an efficient and reversible electrochemical hydrogen storage system based on the nitrogen heterocyclic organic hydrogen carrier, quinoline. Here, the RuNi/NF electrode serves as an electrocatalyst to produce 1,2,3,4-tetrahydroquinoline (THQ) under ambient conditions, utilizing H 2 O as a hydrogen source with up to 99% conversion and 99% selectivity. Quinoline was synthesized with 94% conversion and 92% selectivity within the same solution system. This exceptional performance is attributed to the RuNi alloying effect, which enhances both the affinity of the active hydrogen atom (H∗) in the solution and the activity of Ni 2+ in the catalyst. Furthermore, the RuNi electrocatalyst exhibits excellent catalytic stability. The use of water as a hydrogen source eliminates the need for exogenous hydrogen, ensuring the safety of the process. This study provides an environmentally friendly and safe strategy for hydrogen storage in nitrogen heterocyclic organic carriers. By achieving efficient hydrogenation and dehydrogenation of LOHCs through electrochemical methods, this work not only expands the technical pathways for hydrogen storage but also offers important theoretical and practical insights for the development of future clean energy technologies.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2012
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IF 3.07
Peng Liao,Songhu Yuan,Wenjing Xie,Wenbiao Zhang,Man Tong,Kun Wang
The adsorption kinetics and thermodynamics of nitrogen-heterocyclic compounds (NHCs), pyridine, indole and quinoline, in aqueous solutions on bamboo charcoal (BC), as well as the regeneration of spent BC by microwave radiation, are investigated. BC is produced by incomplete combustion of moso bamboo at high temperature and nitrogen atmosphere. Adsorption kinetics is analyzed using pseudo-first-order and pseudo-second-order as well as Weber–Morris model. The results show that NHC adsorption on BC is predominantly regulated by surface diffusion in initial 1 h followed by intraparticle diffusion in later stage. BC exhibits a strong adsorption affinity to NHCs, and the adsorption isotherms are well described by Freundlich model. Thermodynamic analysis indicates that the adsorption is spontaneous and endothermic. Adsorption site energy analysis illustrates a distribution of adsorption energy, which indicates the heterogeneous sites on BC for NHC adsorption. Furthermore, spent BC with NHC adsorption can be effectively regenerated by MW radiation. The adsorption capacity becomes even higher than that of virgin BC after five times of adsorption–regeneration cycles. This study proves BC is a promising adsorbent for NHC removal in wastewater.
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Journal of Water Process Engineering
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2025
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IF 6.7
Yan Cui,Wenrui Du,Yao Zhang,Jifan Hu,Weiwei Kang
Quinoline is a representative refractory ammonia nitrogen contaminant in coking wastewater, which presents a hazard to the environment and humanity. Thus, effective settlement of quinoline is eagerly required. Nevertheless, existing adsorbents are expensive and inefficient in quinoline adsorption. It is significant to explore a low-cost and efficient adsorbent. Herein an environmental-friendly activated biochar derived from agricultural waste walnut shell was synthesized. Activated biochar displays large surface area, rich pores and high surface activity. The adsorption behavior of activated biochar was tested under static and dynamic adsorption systems. Activated biochar represents excellent adsorption performance and industrial application potential. Under the conditions of 298 K, 650 rpm and pH = 7, the activated biochar's saturated adsorption capacity and equilibrium time for quinoline are 342.56 mg g −1 and 20 min, respectively. After five adsorption-desorption cycles, the adsorption capacity retained 93.43 % of the incipient value, indicating that activated biochar exhibits excellent regeneration performance. Moreover, activated biochar could maintain good adsorption performance in real wastewater. More importantly, using walnut shell as the raw material could save costs and realize resource utilization. The negative Δ G θ and positive Δ H θ values demonstrate that the adsorption process is spontaneous and endothermic, which follows the pseudo-first-order kinetics and fits well with the Langmuir–Freundlich model. This work has a good guiding significance in the domain of sewage purification.
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WATER RESEARCH
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2025
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IF 12.4
Han Li,Jinrui Shi,Tao Fu,Jinwei Liu,Xiangtian Peng,Liangjie Wang,Huifang Sun,Yi Xu,Huazhang Zhao
High-temperature wastewaters can themselves activate peroxydisulfate (PDS) to remove aromatic contaminants via polymerization. This, however, may result in an insufficient carbon source for denitrification during biochemical treatment, and the formed polymers, without a proper reuse method, will be costly to handle as hazardous waste. This study demonstrates that the addition of NaOH can suppress the polymerization of aromatic contaminants, which is observed not only in simulated wastewater but also in actual coking wastewater (ACW). Taking phenol as an example, the formation of phenoxy radical (PhO•) through the reaction between SO 4 •- and phenol is the crucial step for phenol polymerization. The addition of NaOH can convert sulfate radicals (SO 4 •– ) to hydroxyl radicals (HO•), and simultaneously, HO• can quickly consume PhO•. Both processes contribute to the inhibition of phenol polymerization. After treatment with heat/NaOH/PDS, the biodegradability of ACW is significantly enhanced with a relatively low carbon source loss (around 16%). Moreover, Fourier transform-ion cyclotron resonance mass spectrometry analysis indicates that the transformation of polyphenols to highly unsaturated and phenolic compounds is beneficial for the biodegradability improvement of ACW. Therefore, the NaOH/PDS system is an effective way to utilize waste heat and enhance the biodegradability of wastewater.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-12
·
IF 15.7
Yang Liu,Pu Zhongji,Wu Jianping,Liu Xiaofeng,Wang Zhe,Yu Haoran,Wang Liuwei,Meng Yan,Xu Gang,Yang Lirong,Zheng Wenlong
N -oxidation of N -heterocycles is essential in the synthesis of natural products but challenging due to low efficacy and poor regioselectivity. In this study, the N -oxidation selective potential of P450BM3 from Bacillus megaterium for N -heterocyclic compounds is investigated. Here, twelve amino acids located in the active center, including A74, L75, V78, A82, F87, I263, A264, A328, P329, A330, I401, and L437, are investigated by site-saturation mutation. As a result, F87, A264, L75, V78, A328, I401, and L437 are identified as hotspot residues. Subsequently, the combinatorial active-site saturation test/iterative saturation mutagenesis strategy is performed. Using quinoline as a model substrate, the mutant F87G/A264G/A328L exhibits N -oxidation selectivity of up to 99.0%, with a conversion rate of 99.3%. Molecular dynamics simulations uncover a “push-pull” molecular mechanism elucidating the pivotal role of steric factors in determining substrate recognition and N -oxidation selectivity. This study provides an efficient N -oxide synthesis method and insights into P450BM3’s molecular mechanisms.
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ACS Applied Materials & Interfaces
·
2025
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IF 8.2
Wanyu Tian,Lele Qiu,Shuhui Zhou,Jian Xiao,Jing Liang,Fangjing Liu,Yunpeng Zhao
Passivation treatment for perovskite films has constituted an indispensable process in fabricating high-performance perovskite solar cells (PSCs), yet the degradation or dynamic evolution of passivation layers under external stimuli persists as a critical bottleneck impeding commercialization. Here, we develop a silicon phthalocyanine-engineered ammonium cation (SiPc(4HTy)2) that enables perovskite films to resist degradation under thermal stress and meanwhile reinforces the related heterointerfaces in PSCs. The surface passivation strategy based on SiPc(4HTy)2 efficiently reduces surface defects of perovskite films, optimizes energy level alignment, and suppresses ion diffusion, without relying on the formation of two-dimensional perovskite passivation layers. The superior passivation efficacy originates from the solution-processable bulky cation engineering achieved by axially coordinating three-dimensional silicon phthalocyanine. Under the passivation treatment of SiPc(4HTy)2, the power conversion efficiency of PSCs reaches a maximum of 23.55%, mainly due to the improvement of the open-circuit voltage and fill factor. Furthermore, benefiting from the maintenance of the morphology and optoelectronic properties of perovskite films, the related devices still maintain more than 80% of their initial performance after over 1000 h at 85 °C in an inert atmosphere.
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