ACS Omega
·
2023
·
IF 4.1
Ning Shi,Tianlang Zhu,Hongyan Zhang,Hongsheng Huang,Liang Zhou,Ying Liu,Riyang Shu
Catalytic conversion of cellulose into the novel platform molecule 2,5-hexanedione (HXD) is regarded as one feasible approach for high-value utilization of biomass resources. Here, we reported one efficient way of one-pot conversion of cellulose into HXD with high yield of 80.3% in H2O and tetrahydrofuran (THF) mixture within Al2(SO4)3 combined with Pd/C as a catalyst. In the catalytic reaction system, Al2(SO4)3 could catalyze the conversion of cellulose into 5-hydroxymethylfurfural (HMF), and Pd/C combined with Al2(SO4)3 could catalyze the hydrogenolysis of HMF into furanic intermediates such as 5-methylfurfuryl alcohol and 2,5-dimethylfuran (DMF) without causing over-hydrogenation of these furanic intermediates. These furanic intermediates were finally transformed into HXD catalyzed by Al2(SO4)3. Besides, the H2O/THF ratio could significantly influence the reactivity of the hydrolytic furanic ring-opening of the furanic intermediates. The catalytic system also showed excellent performance on the conversion of other carbohydrates (glucose and sucrose) into HXD.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Chenghong Wu,Xiaopeng Chen,Jiezhen Liang,Jiawei Fu,Zhongyao Zhang,Xiaojie Wei,Linlin Wang
The catalytic hydrogenation of dicyclopentadiene (DCPD) is one of the pivotal processes in the production of green high-energy-density liquid hydrocarbon fuels, jet propellent-10 (JP-10). However, the high dependency of the current catalysts on high temperature and pressure, whether the non-noble (>120 ℃, >15 bar) or even the noble catalyst (80 ℃, >7.6 bar), leads to enormous energy consumption and technical challenges in environment and sustainable development. Herein, we prepared a carbon layer wrapped Ni nanoparticles/g-C 3 N 4 catalyst (Ni@C/g-C 3 N 4 ) derived from the in-situ-formed Ni-MOF/g-C 3 N 4 composite. Benefiting from the 53.2 wt% small-sized Ni nanoparticles and nanosheet structure, resulting in high-density accessible active sites (5.38 × 10 20 sites g −1 ) and the mass transfer enhancement, Ni@C/g-C 3 N 4 achieved DCPD hydrogenation under ambient conditions. > 99.9 % DCPD conversion and 98.1 % endo -tetrahydrodicyclopentadiene yield was obtained at 30 ℃, 1 bar, significantly outperforming the benchmark 5 % Pd/C. To the best of our knowledge, it’s the mildest condition for DCPD hydrogenation. Further, comprehensive mechanistic insights were gained from combining means of kinetic investigations, in situ characterization, and theoretical calculations. The discrimination result of 27 kinetic models indicated that DCPD hydrogenation followed the Langmuir-Hinshelwood-Haugen-Watson formulism regarding the reaction between the chemisorbed dihydrodicyclopentadiene (DHDCPD) and dissociatively adsorbed hydrogen as the rate-determining step. In-situ DRIFTS confirm that the norbornene ring is preferentially adsorbed and hydrogenated. The DFT calculations further substantiate the hydrogenation pathway. The present work provides guidance for the development of highly efficient non-noble metal catalysts and opens up an environmental-friendly and economically viable avenue for DCPD hydrogenation.
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ACS Omega
·
2023
·
IF 4.1
Bolin Wang,Yuxue Yue,Yuliang Li,Lu Yu,Hong Tang,Haifeng Zhang,Feng Feng
Imidazolium-based ionic liquid mixtures with [NO3]− and [AlCl4]− anions were used as oxidizing agents for the dissolution of Au, Pd, and Pt metals under mild conditions. The thermodynamic reduction of [NO3]− to [NO] is catalyzed by [AlCl4]− anions and coupled with the oxidation process of noble metals. The developed ionic liquid system for dissolving Au can reactivate the Au0 formed in the deactivation process of the catalyst in vinyl chloride production. This demonstrates the relevance of the here-presented work for technical noble metal recycling.
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ChemSusChem
·
2019
·Vol. 12
·期 17
·3977-3987
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IF 7.804
Qiying Liu,Haiyong Wang,Haosheng Xin,Chenguang Wang,Long Yan,Yingxiong Wang,Qi Zhang,Xinghua Zhang,Ying Xu,George W. Huber,Longlong Ma
Graphical Cellulose conversion into ethanol : Ethanol is obtained through one-pot cellulose hydrogenolysis over graphene-layers-encapsulated nickel catalysts with the aid of H 3 PO 4 in water. This work, for the first time, demonstrates a chemocatalytic approach for a high-yield production of ethanol from biomass using a non-noble metal catalyst. Ethanol is an important bulk chemical with diverse applications. Biomass-derived ethanol is traditionally produced by fermentation. Direct cellulose conversion to ethanol by chemocatalysis is particularly promising but remains a great challenge. Herein, a one-pot hydrogenolysis of cellulose into ethanol was developed by using graphene-layers-encapsulated nickel (Ni@C) catalysts with the aid of H 3 PO 4 in water. The cellulose was hydrolyzed into glucose, which was activated by forming cyclic di-ester bonds between the OH groups of H 3 PO 4 and glucose, promoting ethanol formation under the synergistic hydrogenation of Ni@C. A 69.1 % yield of ethanol (carbon mole basis) was obtained, which is comparable to the theoretical value achieved by glucose fermentation. An ethanol concentration of up to 8.9 wt % was obtained at an increased cellulose concentration. This work demonstrates a chemocatalytic approach for the high-yield production of ethanol from renewable cellulosic biomass at high concentration.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2019
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IF 3.131
Rui Sun,Fangfang Ren,Dong Wang,Yufeng Yao,Zhenghao Fei,Huiwen Wang,Zongtang Liu,Rong Xing,Yukou Du
Design of high performance and low cost electrocatalysts for the oxidation of small organic molecules remains a great challenge for the practical application of direct fuel cells. Herein, a novel composite catalyst composed of PdAu nanoparticles (NPs) uniformly dispersed on the polydopamine functionalized MWCNTs (PDA-MWCNTs) has been synthesized. TEM images indicate that MWCNTs are successfully coated by PDA, and the as-prepared PdAu NPs are homogeneously dispersed on the PDA functional MWCNTs with smaller sizes than those on pristine MWCNTs. Electrochemical tests reveal that PDA-MWCNTs is a promising catalyst carrier for direct ethylene glycol fuel cell (DEGFC), and the PdAu(1:1)/PDA-MWCNTs catalyst displays the highest peak current density among all catalysts towards ethylene glycol oxidation reaction (EGOR) in alkaline medium, with mass activity of 1540.3 mA mg Pd −1 , which is 1.5, 2.6, 9.8, 13.4 and 2.0 times greater than those of PdAu(1:3)/PDA-MWCNTs, PdAu(3:1)/PDA-MWCNTs, Pd/PDA-MWCNTs, Pd/MWCNTs and commercial Pd/C catalysts, respectively. In addition, PdAu(1:1)/PDA-MWCNTs catalyst also exhibits the best stability. These findings are valuable for the development of advanced Pd-based catalysts, which will help promote the industrialization of direct fuel cell.
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JOURNAL OF CATALYSIS
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2019
·
IF 7.723
Lei Yang,Shiyi Yu,Chong Peng,Xiangchen Fang,Zhenmin Cheng,Zhiming Zhou
A series of nonprecious monometallic Ni/AlSBA-15 and bimetallic Ni M (M = Zn, Ga, Cu, or Fe)/AlSBA-15 catalysts were prepared using a urea precipitation method and applied to the semihydrogenation of phenylacetylene. The catalysts were characterized by various techniques, showing that the Ni particle size of catalyst can be tuned by adjusting the Al content, and NiZn and NiGa supported catalysts exhibited geometric and electronic effects that originated from the bimetallic alloy. Among all the catalysts studied, NiZn 3 /AlSBA-15, with a turnover frequency of 10.89 s −1 comparable to that of precious Pd-based catalysts, presented the highest selectivity to styrene (90.3%) at nearly 100% conversion of phenylacetylene in semibatch operation. This catalyst was further evaluated in a continuous fixed-bed reactor for semihydrogenation of a model C 8 aromatic fraction of pyrolysis gasoline (a mixture of phenylacetylene, styrene, ethylbenzene and xylene), which aimed at assessing its practical application of recovering styrene from pyrolysis gasoline. The results showed that at complete conversion of phenylacetylene, the styrene concentration in the product was always kept at a stable level and higher than its initial concentration over 100 h of time on stream, demonstrating high selectivity and good stability of NiZn 3 /AlSBA-15. Finally, the application of NiZn 3 /AlSBA-15 was extended to other phenylacetylene derivatives.
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HIGH PERFORMANCE POLYMERS
·
2019
·
IF 1.584
Xianfeng Que,Zhiming Qiu,Yurong Yan
Benzocyclobutene (BCB) resins have aroused much interest because of their excellent physical and chemical properties. Unfortunately the temperature required to induce cross-linking in typical BCBs is higher than 250°C, which restricts their applications. In this study, a novel cyano-containing BCB-terminated imide monomer was synthesized through the reaction of 1-cyano-5-amino-benzocyclobutene with 4,4′-oxydiphthalic anhydride. This monomer allows a 50–100°C lower curing temperature in comparison with typical BCBs, and it is highly soluble in various solvents and can easily convert to cured film at 150–200°C. Because of the presence of rigid imide group and strong polar cyano group, the cured film exhibits excellent mechanical strength with tensile strength up to 87.8 MPa, high glass transition temperature up to 350°C, low coefficient of thermal expansion (36.9 ppm K−1), and outstanding planarity with the average surface roughness as low as 0.26 nm.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2019
·
IF 4.084
Zhong Dong,Feiyu Li,Qiang He,Xuezhang Xiao,Man Chen,Chuntao Wang,Xiulin Fan,Lixin Chen
The development of cost-effective heterogeneous catalysts for the dehydrogenation of formic acid (FA) is the key challenge for the commercialization of FA as a hydrogen-storage medium. Herein, PdCoNi nanoparticles (NPs) with different element ratios supported on N-doped carbon nanosheets (N-CN) were designed, which exhibit excellent catalytic dehydrogenation performance for FA. Compared with PdCoNi NPs loaded on the carbon nanosheets (CN), the introduction of pyrrolic N to CN induces the formation of ultrafine, monodispersed and amorphous Pd 0.6 Co 0.2 Ni 0.2 NPs with a size of 1.60 nm, which significantly increases the number of active sites and the instant contact between FA and catalysts. The as-prepared Pd 0.6 Co 0.2 Ni 0.2 /N-CN catalyst shows more than 99% conversion and 100% H 2 selectivity at room temperature , with a record-high initial turnover frequency (TOF initial ) of 1249.0 h −1 among non-noble containing Pd-based catalysts, which demonstrates the high potential of Pd 0.6 Co 0.2 Ni 0.2 /N-CN as a practical catalyst for the hydrogen generation from FA.
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JOURNAL OF CATALYSIS
·
2019
·
IF 7.723
Zhaolin He,Jin Liu,Qijun Wang,Meng Zhao,Zhipan Wen,Jun Chen,Devaraj Manoj,Chuyi Xie,Jiangbo Xi,Junxia Yu,Chunyan Tang,Zhengwu Bai,Shuai Wang
Eco-friendly carbocatalyst is extremely desirable in organic catalysis and wastewater treatment. Herein, we reported a one-pot synchronous hydrothermal process to synthesize a highly efficient N doped holey graphene (NHG) carbocatalyst, in which graphene oxide nanosheets are self-assembled, reduced, chemically etched, and simultaneously doped with nitrogen to form a graphene hydrogel in the presence of H 2 O 2 and NH 4 OH. Benefiting from the good hydrophilicity, unique hierarchical porous structure, large specific surface area (322.1 m 2 g −1 ), and high N content (9.77 at. %), the resultant NHG carbocatalyst exhibits an excellent catalytic performance for the hydrogenation of N-containing unsaturated compounds. In 4-nitrophenol reduction reaction, the NHG carbocatalyst delivers a turnover frequency of 3.32 × 10 −2 min −1 . This catalytic activity is superior to that of the commercial Pd/C (5.0 wt%), other previously reported carbocatalysts, and many noble-metal-based catalysts. Furthermore, the molecular structure analysis combined with density functional theory calculations elucidate metal-free catalytic mechanism of hydrogenation reaction for unsaturated chromophore groups in N-containing organic dyes.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2019
·
IF 4.084
Linyan Hong,Qizhi Dong,Qian Qin,Huizi Li,Jian Xie,Gang Yu,Hong Chen
Improved performance and reduced costs are crucial to develop catalysts for direct formic acid fuel cells. In this study, PdBi alloy nanoparticles were synthesized using a facile seed-mediated growth method. The as-synthesized Pd 1 Bi 1 alloy nanoparticles exhibited a large electrochemical surface area (46.3 m 2 g −1 ) and a high mass activity (1.44 A mg −1 ), which was 1.19- and 4.8-fold higher than that of commercial Pd/C catalysts, respectively. The PdBi alloy nanoparticle is a promising catalyst for direct formic acid fuel cells.
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GREEN CHEMISTRY
·
2019
·Vol. 21
·期 10
·2709-2719
·
IF 9.405
Hao Tang,Ning Li,Guangyi Li,Aiqin Wang,Yu Cong,Guoliang Xu,Xiaodong Wang,Tao Zhang
For the first time, gasoline and jet fuel range C7–C8 cycloalkanes and aromatics were selectively synthesized by the alcoholysis of poly(ethylene terephthalate) (PET) waste, followed by solvent-free hydrogenation and hydrodeoxygenation (HDO). It was found that methanol is highly reactive for the alcoholysis of PET waste. In the absence of any catalyst, a high yield of dimethyl terephthalate (97.3%) was achieved under mild conditions (473 K, 3.5 h). Dimethyl terephthalate exists as a solid and can be automatically separated from methanol with a decrease in temperature. Subsequently, dimethyl terephthalate was liquefied to dimethyl cyclohexane-1,4-dicarboxylate by hydrogenation over noble metal catalysts. Among the investigated catalysts, Pt/C exhibited the highest activity. Finally, the dimethyl cyclohexane-1,4-dicarboxylate as obtained was further hydrodeoxygenated to C7–C8 cycloalkanes and aromatics that can be used as gasoline or additives to improve the densities (or volumetric heat value) and sealabilities of current bio-jet fuels. Bimetallic Ru–Cu/SiO2 was found to be a promising HDO catalyst. According to the characterization results, the excellent HDO performance of Ru–Cu/SiO2 can be explained by the formation of smaller Ru–Cu alloy particles during the catalyst preparation. In real applications, dimethyl cyclohexane-1,4-dicarboxylate can also be simultaneously hydrodeoxygenated with biomass derived oxygenates to produce jet fuel with a suitable content of cycloalkanes and aromatics.
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ChemCatChem
·
2019
·Vol. 11
·期 11
·2676-2682
·
IF 4.495
Qinglin Yuan,Wanbing Gong,Yixing Ye,Jun Liu,Yue Lin,Chun Chen,Haimin Zhang,Pengfei Li,Weiren Cheng,Xiangjun Wei,Changhao Liang
Graphical Coupling reaction : A novel Pd/BiOCl catalyst is designed to catalyze benzaldehyde for high-selectively synthesizing benzoin ethyl ether utilizing the nucleophilic action of Cl − ions. DFT calculations and experimental evidences demonstrated the key role of dissociated Cl − ions with Pd NPs by suppressing the dissociation of Cl − ions and changing the reaction pathway. Exploring novel catalyst supports with unique performance creates more opportunity for transforming organic chemicals in heterogeneous catalysis. In this paper, BiOCl is first presented as an effective support for Pd nanoparticles (NPs) toward application in the coupling reaction of benzaldehyde. The Cl − ion dissociates from BiOCl, which forms nucleophile with Pd nanoparticles; this is key for the one-step synthesis of benzoin ethyl ether, the conversion and selectivity of which can reach to 100 % and 97.9 % at 100 °C, respectively. DFT calculations reveal that Cl − ions can be stabilized by stronger Bi−Cl bonds through doping of Fe ions in substituting Bi sites in BiOCl. The parallel catalytic evaluation using Pd/Fe-doped BiOCl catalyst shows the suppression of coupling reaction, conversely, demonstrating the crucial role of nucleophile. This work provides new insights into support tailoring for the synthesis of vital organic chemicals in heterogeneous catalysis by changing chemical reaction pathway.
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