APPLIED SURFACE SCIENCE
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2021
·
IF 6.707
Li Zhang,Xuerui Yang,Runsheng Zhou,Sen Lin,Lei Zhou
In this study, Ni/Co layered double hydroxide (Ni/Co-LDH) with uniform flake structure was synthesized successfully as an effective activator in the carbamazepine (CBZ) degradation by peroxymonosulfate (PMS). Our results indicated that Ni/Co-LDH possessed a high specific surface area (72.9942 m 2 /g) and exhibited great activation performance, in which 100% CBZ removal could be achieved within 300 s under neutral conditions with 5 mg/L Ni/Co-LDH and 0.3 mmol/L PMS. In addition, the crystal structure and morphology of the prepared Ni/Co-LDH kept unchanged during degradation cycles. X-ray photoelectron spectroscopy (XPS) analysis and free radical identification experiment speculated that the cycle of Ni 2+ /Ni 3+ and Co 2+ /Co 3+ on Ni/Co-LDH surface were responsible for efficient HO•/SO 4 •− generation from PMS. Based on identified products through high resolution mass spectrometry (HR-MS), it was proposed that the degradation pathway of CBZ was a heterozygous process involving deamidation, hydroxylation and electron transfer. The ECOSAR calculation results indicated the toxicity of some products was still at very toxic level, thus certain attention should be paid to the toxicity of intermediates in the process of treating pollutants in water.
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ACS Catalysis
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2021
·
IF 13.084
Ting Wang,Yuebing Xu,Yufeng Li,Lei Xin,Bing Liu,Feng Jiang,Xiaohao Liu
Conversion of syngas into aromatics via the Fischer–Tropsch (FT) route provides a promising way to supply the value-added chemicals. However, it is still a great challenge to achieve controllable aromatics selectivity with good stability. Herein, we report the Na-mediated bimetallic Fe–Ni catalyst simply particle mixed with HZSM-5, which can boost the stable and selective production of aromatics from the syngas. In detail, FeNiOx(5:1)-0.41Na exhibits quite stable catalytic activity with notably higher selectivity to light α-olefins (C2=–C4=) compared to α-Fe2O3-0.75Na. Various characterizations suggest that an appropriate addition of Ni with Na substantially regulates iron carbide formation and suppresses carbon deposition owing to the electron donation of Fe to Ni reducing CO adsorption and dissociation. Interestingly, extra Na results in remarkably increased selectivity to C1o–C4o, despite the fact that Na shows the ability to suppress hydrogenation. Both characterizations and density functional theory (DFT) calculations demonstrate that the addition of Na weakens the Fe–Ni interaction and reduces electron transfer from Fe to Ni, which promotes C1o–C4o formation as Ni tends to reflect its intrinsic catalysis. DFT calculations confirm that the adsorbed CH2 species at the Ni–Fe interface prefers to undergo coupling to form C2H4, and the formed C2H4 spontaneously desorbs from the surface, indicating that the formation of lower olefins is favorable and further chain growth is inhibited. This could be attributed to the fact that the accumulated electron at the Ni–Fe interface weakens the binding strength of CH2 and C2H4 species because of electronic repulsion. Furthermore, the effects of FT product distribution on aromatics formation were also investigated. FeMnOx(5:1)-0.40Na produces longer olefin-rich hydrocarbons in C5+ owing to oxygen vacancy-assisted CO dissociation, leading to highly branched monocyclic aromatics and faster HZSM-5 deactivation because of increased coking from the isomerization–hydrocracking of long hydrocarbons. In contrast, FeNiOx(5:1)-0.41Na-HZSM-5 produces major light aromatics about 65.7% including toluene, ethyl-benzene, and xylene in total aromatics with about 98.6% aromatics in the liquid phase, which benefits from the fact that FeNiOx(5:1)-0.41Na makes shorter hydrocarbons in C5+ and/or Ni metal has a strong ability of H2 dissociation to provide atomic H spillover onto HZSM-5. Thus, HZSM-5 also shows improved stability. Note that the mixed catalysts with a high Na content indicate a substantial Na+ migration to increase light α-olefins in the gas phase owing to suppress H-transfer reaction. This study provides deep insights into how to develop stable and selective iron-based catalysts for the production of FT products and its further conversion into value-added light aromatics.
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CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Jingwen Zhang,Chuchu Cheng,FangShu Xing,Cheng Chen,Caijin Huang
Engineering semiconductor materials with vacancies and co-catalysts is a valid method to improve their photocatalytic performance. Herein, we prepared S vacancies-rich Mn 0.3 Cd 0.7 S nanorods modified with β-Ni(OH) 2 nanoparticles through solvothermal and co-precipitation strategies. The as-obtained 0D/1D β-Ni(OH) 2 /Mn 0.3 Cd 0.7 S nanorods exhibit excellent visible-light H 2 -production activity up to 71.09 mmol g −1 h −1 , 5.23 times higher than pure Mn 0.3 Cd 0.7 S and better than 1 wt% Pt/Mn 0.3 Cd 0.7 S and most reported Mn x Cd 1−x S-based catalysts. The apparent quantum yield reaches 46.68% at λ = 420 nm. We found that the presence of S vacancies and β-Ni(OH) 2 enhances the transfer/separation of photogenerated carriers and increases reaction sites, which is beneficial to photocatalytic H 2 -production reaction. This work proposes a new idea for the application of metal hydroxide co-catalysts and S vacancies in sulfide materials for photocatalytic H 2 production.
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Journal of Materials Research and Technology-JMR&T
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2021
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IF 5.039
Weiwei Zhang,Tianyong Mei,Baosong Li,Lu Yang,Shengsong Du,Yicheng Miao,Hongqiang Chu
In this work, Ni/diamond composite coatings have been synthesized by electrodeposition in direct current mode. The effects of mechanical and ultrasonic agitations on the microstructural, surface characteristics and electrochemical properties have been comparatively investigated by various methods. Results show that diamond nanoparticles have been evenly dispersed in Ni metallic matrix, which could reinforce their performances. The coatings prepared under ultrasonic and mechanical agitation both exhibit compact, dense and hill-valley like morphology with pyramid-like nickel crystallite grains. The relative texture coefficient (RTC) values show that the preferred orientation of the Ni/diamond coating was (200) texture. From 3 to 5 A dm −2 , the crystallite sizes of ultrasonic conditions were 59.2–81.7 nm, which were smaller than 76.3–83.2 nm of magnetic agitations. The average roughness ( R a = 78.9–133 nm) of ultrasonic-assisted coatings were lower than 103–139 nm of magnetic conditions. The mechanism of the co-electrodeposition process was proposed. Electrochemical impedance spectroscopy (EIS) results illustrate that the ultrasonic-assisted electrodeposited Ni/diamond coating has better corrosion resistance than that prepared under mechanical stirring conditions. The Ni/diamond composite coatings could be applied as protective materials in harsh mediums.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2021
·Vol. 168
·期 3
·034516
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IF 4.316
Kai Li,Yafeng Jin,Wenming Gao,Shoucai Xue,Ming Zhang
A critical issue for massive production of metal-supported solid oxide fuel cell is cathode processing due to the contradicting of the metal support and the cathode with regard to the sintering atmosphere. Herein, LSM-BSCF (La0.8Sr0.2MnO3-δ coated Ba0.5Sr0.5Co0.8Fe0.2O3-δ) cathodes on Ni-Fe alloys supported SOFCs (NF-SOFCs) are fabricated by an ex situ sintering approach and electrochemical evaluation in humidified H2 fuel. The ex situ sintering of cathodes on NF-SOFCs are performed at 1050 °C in air with metal oxide support consisted of NiO and 10 at% Fe2O3, and then the oxide support is reduced in situ into Ni-Fe alloys during testing. Cross-section microstructure analysis shows clear evidence that each layer is well adhered to each other after reduction and the suitable microstructure of ex situ sintered cathode is observed after sintering at 1050 °C. In the single-cell test, a higher peak power density is achieved for NF-SOFC with ex situ sintered LSM-BSCF in comparison with in situ sintered cells, revealing a beneficial effect of ex situ sintered cathode on cell performance. The durability measurement and post-test analysis confirm the sufficient adherence and mechanical stability between ex situ sintered LSM-BSCF cathode and GDC (Ce0.9Gd0.1O1.95) electrolyte. The successful electrochemical characterizations of NF-SOFCs with ex situ sintered LSM-BSCF cathode confirm the applicability of the novel sintering procedure.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
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IF 8.128
Zhenlin Ma,Rong Zheng,Yu Liu,Yulong Ying,Weidong Shi
Recently, carbon nanotubes (CNT)-based interconnected architectures exhibit promising prospects in supercapacitors due to their flexibility and high electrical conductivity. Herein, a three-dimensional (3D) interconnected network structure combined with conductive carbon nanotubes interpenetrating MOFs-derived Co-Ni-S composite spheres (Co-Ni-S/CNTs) was synthesized. Such 3D interconnected architecture significantly leads to a favorable electronic structure, fast charge-transfer capacity, and more pseudocapacitive. The Co-Ni-S/CNTs-based hybrid electrode exhibits an extraordinary specific capacitance of 540.6C g −1 at 1 A g −1 and competitive rate performance (capacity retention rate of 69.9% when the current density increases to 10 times). Subsequently, a hybrid supercapacitor is assembled using Co-Ni-S/CNTs as the positive electrode and commercial activated carbon as negative electrode. The device delivers a high energy density of 63.5 W h kg −1 at 800 W kg −1 and keeps 83.0% initial capacitance retention after 10,000 cycles. The encouraging performances demonstrate the significant contribution of the 3D interconnected architecture for the future energy storage.
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PubMed
高影响因子
Small
·
2021
·Vol. 17
·期 36
·2102002
·
IF 13.281
Hong Li,Xinxin Shu,Peiran Tong,Jihui Zhang,Pengfei An,Zhengxing Lv,He Tian,Jintao Zhang,Haibing Xia
In this work, Fe–Ni alloy nanoclusters (Fe–Ni ANCs) anchored on N, S co-doped carbon aerogel (Fe–Ni ANC@NSCA catalysts) are successfully prepared by the optimal pyrolysis of polyaniline (PANI) aerogels derived from the freeze-drying of PANI hydrogel obtained by the polymerization of aniline monomers in the co-presence of tannic acid (TA), Fe 3+ , and Ni 2+ ions. In addition, the optimal molar ratio of the TA, Fe 3+ , and Ni 2+ ions for synthesis of Fe–Ni ANC@NSCA catalysts are 1:2:5, which can guarantee the formation of carbon aerogel composed of quasi-2D porous carbon sheets and the formation of high-density Fe–Ni ANCs with an ultrasmall size between 2 to 2.8 nm. These Fe–Ni ANCs consisting of N 4 –Fe–O–Ni–N 4 moiety are proposed as a new type of active species for the first time, to the best of the authors’ knowledge. Thanks to their unique features, the Fe–Ni ANC@NSCA catalysts show excellent performance in oxygen reduction reaction with a half-wave potential ( E 1/2 ) of 0.891 V and oxygen evolution reaction (260 mV @ 10 mA cm −2 ) in alkaline media as bifunctional catalysts, which are better than the state-of-the-art commercial Pt/C catalysts and RuO 2 catalysts. Moreover, Zn–air battery assembled with the Fe–Ni ANC@NSCA catalysts also shows a remarkable performance and exceptionally high stability over 500 h at 5 mA cm −2 .
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PubMed
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JOURNAL OF THE ENERGY INSTITUTE
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2021
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IF 6.186
Yunwu Zheng,Jida Wang,Donghua Li,Can Liu,Yi Lu,Xu Lin,Zhifeng Zheng
To improve the quality of bio-oil and minimize coke formation, ex-situ catalytic biomass pyrolysis vapor upgrading to high-grade bio-aromatic and phenol compounds with Py-GC × GC/MS at different nickel-to-copper ratios was investigated. At the same time, the deoxygenation efficiency, structure-activity relationship, deactivation mechanism and possible pathways between combined mono- and bimetallic catalysts were also demonstrated. Ni and Cu species could be well dispersed, and the HZSM-5 support maintained the MFI crystal structure after bimetallic Ni–Cu modification, but the surface area, pore volume, and total acidity decreased. Bimetallic Ni–Cu catalysts showed better deoxygenation efficiency than monometallic catalysts, which had more advantages in the preparation of aliphatic hydrocarbons (29.86%) than mono- and bimetallic catalysts, which favored the production of aromatics (28.89%). Higher-Ni-loading catalysts promoted the formation of aliphatic hydrocarbons, aromatics and alkanes due to decarboxylation, decarbonylation and aromatization reactions, and higher-Cu-loading catalysts enhanced the olefin and phenol yields due to dehydration and demethylation reactions. Overall, the highest yields of bio-aromatic compounds and phenols were46.78% and 36.34%, respectively, at Ni-to-Cu ratios of 1:1 and 1:2, due to the high total acid amount and suitable average pore size for bio-aromatics and the low acidity and large pore size for phenols. The bimetallic Ni–Cu catalyst significantly increased the quality of bio-oil and reduced coke deposition.
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MATERIALS CHEMISTRY AND PHYSICS
·
2021
·
IF 4.094
Xiaorui Zhang,Yu Mei,Hao Cheng,Jianfeng Ma,Fang Zhu,Sridhar Komarneni
NiO and CeO 2 composite metal oxides (NiO–CeO 2 ) were synthesized by sol-gel method to investigate a degradation system by persulfate (PS) activation with the assistance of visible light (Vis). The phase composition of NiO–CeO 2 was detected by X-ray diffraction (XRD), the morphology of NiO–CeO 2 was characterized by scanning electron microscope (SEM), and the result of X-ray photoelectron spectroscopy (XPS) proved the element composition and valence state of the NiO–CeO 2 . In the Vis/PS/NiO–CeO 2 system, the degradation rate of Orange II using a concentration of 50 mg/L was as high as 90% in 15 min but it increased to as high as 99% in 60 min. Mechanism studies have shown that the combination of NiO and CeO 2 generated more oxygen vacancies , and activated persulfate to generate active oxygen species. Moreover, the effects of visible light , persulfate concentration and pH were evaluated, and the results showed that the participation of visible light and persulfate could significantly increase the degradation efficiency of Orange II, but pH had little effect on the degradation. Quenching experiments and detection by ESR showed that O 2 ‾, •SO 4 ‾, •OH, and 1 O 2 all contribute to the removal of Orange II. In addition, the recovery and reuse properties of NiO–CeO 2 may lead to sustainable treatment of wastewater.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2021
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IF 5.816
Xingchen Gao,Kaixin Lu,Jianjun Chen,Jie Min,Deliang Zhu,Manlin Tan
The design and manufacture of effective non-noble metal catalysts for the H 2 evolution reaction (HER) are urgent for realizing a cost-effective hydrogen production . We report herein on flower-like structures consisting of NiCoP–CoP heterostructural nanowires grown directly on the hierarchically porous nickel framework (NiCoP–CoP/Ni/NF) to achieve a highly efficient HER in alkaline solution (1.0 M KOH). The NiCoP–CoP/Ni/NF is synthesized by electrodeposition of porous Ni layers on Ni foam, followed by simple hydrothermal reaction and phosphorization. For HER, the binder-free NiCoP–CoP/Ni/NF electrode can reach 10 mA cm −2 current density at a quite low overpotential of 49 mV, because of the combination of porous Ni layers and highly active NiCoP–CoP nanowires. In addition, the NiCoP/CoP heterostructures exhibited remarkable stability under the long-term durability test. This work provides a new strategy that combines electrodeposition and hydrothermal reaction to synthesize effective HER catalysts.
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JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
·
2020
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IF 3.905
Tong Li,Hao Li,Guoming Huang,Xinhui Shen,Siqi Wang,Chunli Li
The development of a carbon-based catalyst for selective transformation of renewable lignin to value-added chemicals is a fascinating chemical upgrade route. In this study, the highly efficient Ni/C catalysts derived from waste biomass tar was fabricated for selective hydrogenation-transalkylation (HTTA) of guaiacol to 1-methyl-1,2-cyclohexanediol. Carbonization temperatures and activators can be used to regulate the contents of oxygen-containing functional groups on carbon surface, which further affect the catalytic performance. Results showed that the Ni/C-K-800 catalyst with KOH as activator and 800 ℃ as carbonization temperature exhibited the excellent catalytic performance (about 100 % conversion) for the guaiacol transformation at 220 ℃, 2 MPa H 2 for 2 h, and the final product could be stably controlled at 1-methyl-1,2-cyclohexanediol. Main reaction pathway of guaiacol over Ni/C catalyst was proposed: 1) conversion of guaiacol to 1-methyl-1,2-cyclohexanediol through transalkylation and hydrogenation of benzene ring; 2) transform of 1-methyl-1,2-cyclohexanediol to cyclohexanol through direct hydrogenolysis. Furthermore, biomass tar-derived carbon support has good resistance towards carbon accumulation on Ni metals. These findings can provide a basis for designing green and efficient catalyst derived from biomass tar for biomass upgrading.
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JOURNAL OF THE CHINESE CHEMICAL SOCIETY
·
2020
·Vol. 68
·期 4
·582-591
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IF 1.554
Changzhou Chen,Peng Liu,Haihong Xia,Minghao Zhou,Jianchun Jiang
There is an urgent need to develop a selective hydrogenolysis of C aryl -O bonds in lignin to produce valued-added chemicals and fuels. Recently, hydrogen has been used in the hydrogenation reaction, which hides inevitable danger and is not economical. Therefore, isopropanol, as a hydrogen-donor solvent, is employed for aryl ether hydrogenolysis in lignin models over nickel supported on a carbon nanotube (CNT). Except for aromatic ether (4-O-5), the Ni/CNT catalyst is also found to be suitable for alkyl-aryl ether (α-O-4 and β-O-4) cleavage in control experiments. The physicochemical characterizations were carried out by means of H 2 -temperature-programmed reduction, X-ray diffraction, transmission electron microscopy, and X-ray photoelectron spectroscopy analyses. The catalyst can be magnetically recovered and efficiently reused for five consecutive recycling tests in the transfer hydrogenation of aromatic ethers. A mechanism study indicated that the hydrogenolysis cleavage of the ether bond is the first step in the reaction process, and hydrogenation of aromatic rings is only a successive step in which phenol and benzene are intermediate states and are then further hydrogenated. Furthermore, it has been demonstrated that aryl groups play an important role in the hydrogenation of phenol in the competitive catalytic hydrogenation reaction of phenol.
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