APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Shujuan Lv,Ying Deng,Qian Liu,Ziqi Fu,Xiaobin Liu,Minghui Wang,Zhenyu Xiao,Bin Li,Lei Wang
The hollow materials with open structure can accelerate the mass transfer and bubble release rate, which have attracted tremendous attention for electrocatalytic water splitting. In this work, a unique tri-metal phosphide open nanotube structure [FeCoNiP@carbon quantum dots, FCNP@CQDs] is firstly fabricated by a selected etching and phosphating process with a MIL-88A@CQDs (MIL stands for Material of Institute Lavoisier) as the precursor. Benefiting from their open structure, FCNP@CQDs exhibit excellent catalytic performance. In alkaline seawater solution, a low overpotential of 268 mV is required to reach 20 mA cm −2 current density for oxygen evolution reaction, while the η 20 of hydrogen evolution reaction is 150 mV. The FCNP@CQDs//FCNP@CQDs electrolyzer requires a voltage of 1.61 V to reach 10 mA cm −2 . The integrated strategy of CQDs-doping and construction of hollow open structures may open a new and relatively unexplored path for fabricating high-performance seawater splitting catalysis.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2022
·
IF 6.371
Wenjing Zhao,Peng Wang,Fan Zhang,Yinshen Liu,Xuan Jin,Shijun Yuan,Qi Fan,Xing Guo,Qingyu Xu
Cation-disordered rock-salt cathodes have attracted extensive attention due to their high capacity and energy density . However, the excessive redox reaction of O 2- causes a severe impairment of Ni capacity and the release of O 2 , leading to the poor cycle stability and voltage decay for Li-Ni-Nb-O cathodes. In our work, the oxyfluoride compounds Li 1.23 Ni 0.3 Nb x Fe y O 2- z F z with various doping concentrations of Fe and F are successfully synthesized by solid state reaction using high-energy ball milling. Apart from observing the plateau at around 4 V with the redox reaction of Ni, a new plateau at approximately 2.6 V is observed due to the redox reaction of Fe. The doping of Fe on Nb increases the discharge capability and the co-doping of F on O further improves cycle stability. With the optimized doping amount of Fe ( y = 0.16) and F ( z = 0.15), Li 1.23 Ni 0.3 Nb 0.30 Fe 0.16 O 0.85 F 0.15 can deliver a discharge capacity of 347.1 mAh/g at a current density of 20 mA/g after the activation process in subsequent cycles. After 20 cycles at 20 mA/g, the capacity retention is 181.6 mAh/g, and after 100 cycles at 50 mA/g, the discharge capacity remains 102.2 mAh/g.
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ACS Nano
·
2023
·
IF 17.1
Wanbing Gong,Xin Mao,Jifang Zhang,Yue Lin,Haimin Zhang,Aijun Du,Yujie Xiong,Huijun Zhao
In theory, electrocatalysts in their metallic forms should be the most stable chemical state under cathodic potentials. It is known that the highly dispersed nanoparticle (NP) types of electrocatalysts often possess higher activity than their bulk counterparts. However, facilely and controllably fabricating well-dispersed nonprecious metal NPs with superior electrocatalytic activity, selectivity, and durability is highly challenging. Here, we report a facile reductive pyrolysis approach to controllably synthesize NiCo alloy NPs confined on the tip of N-doped carbon nanotubes (N-CNTs) from a bimetal-MOF precursor. The electrocatalytic performance of the resultant NiCo@N-CNTs are evaluated by a wide spectrum of nitroarene reductive coupling reactions to produce azoxy-benzenes, a class of precious chemicals for textile, food, cosmetic, and pharmaceutical industries. The superior electrocatalytic stability, full conversion of nitroarenes, >99% selectivities, and >97% faradic efficiencies toward the targeted azoxy-benzene products are readily attainable by NiCo@N-CNTs, attributable to the alloying-induced synergetic effect. The presence of a CNT confinement effect in NiCo@N-CNTs induces high stability. This added to the metallic states of NiCo empowers NiCo@N-CNTs with excellent electrochemical stability under reductive reaction conditions. In an effort to enhance the energy utilization efficiency, we construct a NiCo@N-CNTs||Ni(OH)2/NF two-electrode electrolyzer to simultaneously reduce nitrobenzene at the cathode and 5-hydroxymethylfurfural with >99% yields for both azoxy-benzene and 2,5-furandicarboxylic acid.
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PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Haopeng Jiang,Mengyang Xu,Xiaoxue Zhao,Huiqin Wang,Pengwei Huo
The electron density on the catalyst surface has a great influence on the multi-electron transport process of photocatalytic reduction of CO 2 . In this work, hierarchical Cu 2 O/Ni-MOF composite photocatalyst with local surface plasmon resonance (SPR) properties was prepared by simple hydrothermal and water bath methods. Through DRS, XPS and AES tests found that the SPR of Cu 0 expanded the light absorption , provided hot electrons for the reaction system, and greatly improved the photocatalytic activity in coordination with the hierarchical structure and heterostructure. In the absence of sacrificial agent, the CO yield of 30%-Cu 2 O/Ni-MOF was 4.1 times of Cu 2 O (5.32 μmol/g) and 11.1 times of Ni-MOF (1.95 μmol/g), respectively. Then, the possible photocatalytic reaction path was simply speculated based on in-situ FT-IR. In conclusion, the hierarchical structure, heterostructure and SPR effect accelerate the kinetics of Cu 2 O/Ni-MOF photocatalytic reaction, thus improving its photocatalytic activity.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Jiasheng Wang,Ying Zhang,Xiaonan Xu,Ming Bao
Halogenated arylamines are important intermediates for the synthesis of dyes, pesticides, herbicides, and other chemicals. One important way to prepare halogenated arylamines is catalytic hydrogenation of halogenated nitroarenes. Ni-based catalysts have been used in the hydrogenation of halogenated nitroarenes but suffer from low activity and dehalogenation side reaction. In this paper, Ni–CeO2/SiO2 heterojunction catalyst with a “raisin-bun” structure was prepared by reverse microemulsion. A built-in electric field and more oxygen vacancies were formed due to electron transfer from Ni to CeO2 as a result of their work function difference. The built-in electric field leads to the heterolytic cleavage of H2, thereby improving the hydrogenation activity. Oxygen vacancies preferentially adsorb and activate nitro groups, inhibiting the dehalogenation side reaction. Through the cooperation of built-in electric field and oxygen vacancy, synchronous enhancement of the activity and selectivity is obtained successfully. This finding provides a new view for the design of non-noble metal-based catalysts with high activity and selectivity.
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PubMed
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Tengfei Zhang,Peng Zheng,Fangna Gu,Wenqing Xu,Wenxing Chen,Tingyu Zhu,Yi-Fan Han,Guangwen Xu,Ziyi Zhong,Fabing Su
Hydrogenation of CO 2 into CH 4 is an effective strategy for dealing with CO 2 -relevant environmental problems. Since the CO 2 methanation reaction involves multiple electron transfers and various C1 intermediates, improving the reaction rate at each step is critical to accelerating the entire reaction. Here, we report a dual-active-site tandem catalyst (Ru 1 Ni/CeO 2 ) composed of Ru single atoms (Ru 1 ) and Ni nanoparticles , which can effectively convert CO 2 to CH 4 , showing ∼90% CO 2 conversion and ∼99% CH 4 selectivity at 325 °C, much higher than those of the Ru 1 /CeO 2 and Ni/CeO 2 catalysts. Experimental and theoretical calculation results reveal that Ru 1 is extremely active for converting CO 2 to CO, while the Ni site is highly efficient for the subsequent sequential CO to CH 4 reaction step. The coexistence of the Ru 1 and Ni sites significantly boosts the overall reaction. This work offers a promising strategy for the rational design of efficient multisite tandem catalysts.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Yang Tang,Fan Liu,Wenqian Liu,Shaoli Mo,Xiaohong Li,Daxiang Yang,Yijun Liu,Shu-Juan Bao
Hydrogen evolution reaction (HER) electrocatalysts capable of long-term operation under high current densities are key to the industrialization of water-splitting technology. Although numerous efforts have been devoted to expose active sites sufficiently while increasing the intrinsic catalytic activity, effects of non-kinetic factors on catalytic efficiency have not yet been comprehensively investigated. Herein, multifunctional carbon-armored nickel nanoparticles (NC@NiNPs) were fabricated using an in-situ polymer encapsulation method for use as a HER electocatalyst. NC@NiNPs exhibited low overpotential (74 mV at 10 mA cm -2 ), low Tafel slope (85.49 mV dec -1 ) and excellent stability (over 260 h at 1400 mA cm -2 ). Surprisingly, although the intrinsic activity of NC@NiNPs was lower than that of commercial 20 % Pt/C, NC@NiNPs provided markedly greater current density than 20 % Pt/C as the operating voltage was increased. This result implied that non-kinetic factors influenced the HER process, prompting this investigation to identify these unknown factors.
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FUEL PROCESSING TECHNOLOGY
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2022
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IF 8.129
Yiwei Tang,Junyan Fu,Yicong Wang,Haixin Guo,Xinhua Qi
Hydrogenation of levulinic acid to γ-valerolactone is one of the important reactions for conversion of biomass into renewable fuels and chemicals. Ni-Zn non-noble bimetallic catalysts supported on ordered mesoporous carbon (Ni-Zn@OMC) were prepared by one-pot solvent evaporation induced self-assembly (EISA) method and used for hydrogenation of levulinic acid to γ-valerolactone (GVL) in water. A GVL yield of 93% was obtained over bimetallic Ni 1 -Zn 1 @OMC catalyst at 180 °C in 90 min reaction time, with a turnover frequency (TOF) of 686.4 h −1 . Compared with Ni@OMC, the incorporation of Zn metal leads to the formation of Ni-Zn alloy and high dispersion of Ni particle on the catalyst surface . NiO sites on the catalysts lowered competitive adsorption between H 2 and levulinic acid on Ni 0 sites, as well as the Ni-Zn alloy is beneficial to the activation of carbonyl group in levulinic acid, and they synergistically promote the hydrogenation of levulinic acid to 4-hydroxyvaleric acid (4-HVA). Zn content in the catalyst influences both the activity of Lewis acid sites and the ratio of Lewis acid to Brønsted acid sites, and the active sites of Ni δ– Zn δ+ can facilitates the weakening and cleavage of C-O in 4-HVA, both of them are beneficial to the dehydration of 4-HVA to GVL.
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Catalysts
·
2023
·Vol. 13
·期 2
·298
·
IF 3.9
Haoting Yan,Yongwang Ren,Renkun Zhang,Feixiang Chang,Qinhong Wei,Jing Xu
It is a challenging task for selective hydrogenation of cinnamaldehyde (CAL) to hydrocinnamaldehyde (HCAL) without additional by-product formation. In this work, a La2O3supported high Ni content nanoparticle catalyst was prepared for CAL selective hydrogenation. Meanwhile, Co-La2O3catalysts were used as a reference catalyst. XRD, TEM, STEM-HAADF, XPS, and H2-TPR measurements were used to investigate the physicochemical properties of Ni-La2O3catalysts. The experimental results confirmed that the CAL conversion and HCAL selectivity were effectively promoted with the increase of Ni loading amounts. At a Ni/La molar ratio of four, a high HCAL selectivity of 87.4% was obtained at a CAL conversion of 88.1% under mild reaction conditions. The catalyst was recycled five times without activity loss. Combined with various characterizations, it could be inferred that the good hydrogen adsorption and dissociation capacity of Ni and the presence of a certain amount of oxygen vacancies on the La2O3support have a positive effect on the improvement of HCAL selectivity. This work provided an effective path to design transition-metal-based supported oxide catalyst for the cinnamaldehyde hydrogenation to hydrocinnamaldehyde.
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POLYMER DEGRADATION AND STABILITY
·
2022
·
IF 5.204
Yan Lv,Juguo Dai,Long Xia,Lili Luo,Yiting Xu,Lizong Dai
To avoid potential ecological and health problems caused by phosphorus-based flame retardants, a novel phosphorus-free PBA-Salen-Ni flame retardant is successfully synthesized in this work. In a nutshell, boron-containing metal complexes are prepared by nickel salts and chelating PBA-Salen molecule (PBA: p -phenylenediboronic acid). While the obtained material inherently has good compatibility and can endow polymers with good flame retardant properties at low addition levels. Besides, the char shielding layer and the “labyrinth effect” of the special porous char layer structure formed after the combustion of EP/PBA-Salen-Ni retard the transfer of volatile products, giving EP excellent smoke suppression properties. The results show that the limiting oxygen index value of the EP/PBA-Salen-Ni composites is increased from 25.6% (pure EP) to 30.5%, and it can pass the UL-94 V-0 rating when the addition amount is only 5wt%. Particularly, compared with pure EP, the total smoke production (19.9 m 2 ) and peak heat release rate (859.6 kW m −2 ) of EP/PBA-Salen-Ni composites are reduced by 36% and 33%, respectively. Therefore, this work provides a new idea for the rational design of phosphorus-free flame retardants that are mainly on condensed phase flame retardancy and have a good smoke suppression effect.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Wen-Jian Yang,Li-Hui Yang,Han-Jun Peng,Si-Hao Lv,Hafiz Muhammad Adeel Sharif,Wei Sun,Wei Li,Cao Yang,Hui Lin
Electroreduction removal of nitrate (NO 3 – -N) is considered as a promising approach to solve its adverse effects on environment and human health, where efficient and cheap catalysts are required. Perovskite-based catalysts showed a versatile catalytic ability for wide range of redox reactions, but seldom applied for NO 3 – -N reduction. Herein, four perovskite oxide cathodes, LaMO 3-δ (M = Fe, Co, Ni and Cu) were prepared and used for the reduction of NO 3 – -N. The Ruddlesden-Popper (RP) type La 2 CuO 4 exhibited the best NO 3 – -N catalytic activity among the four perovskite oxide cathodes, with a removal rate of 11.7 × 10 -3 min −1 . The high selectivity of NH 4 + -N (82.4 ± 2.2%) indicated that NH 4 + -N was the main final product for NO 3 – -N electroreduction at La 2 CuO 4 cathode, but 100% of N 2 selectivity could be obtained with addition of 1000 and 1500 mg/L Cl - as the electro-assisted chlorination process. The mechanism of NO 3 – -N electroreduction occurred by both electron- and H*-mediated pathway, and the oxygen vacancies and redox cycle of Cu(I)-Cu(II)-Cu(I) were proposed as the accommodation sties and direct electron sources for NO 3 – -N reduction. Generally, this study opens a novel avenue for the development of earth-abundant, cost-effective catalyst with effective NO 3 – -N electroreduction.
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EcoMat
·
2022
·Vol. 4
·期 2
·e12164
·
IF 12.213
Chaoyu Lin,Gan Luo,Huiqin Zhou,Anlin Feng,Li Zeng,Qingyang Li
An amorphous Ni nanoparticles-loaded ZnO nanowire array is controllably constructed on stainless steel mesh through combined electrodeposition and hydrothermal reaction. Its nano-arrayed structure not only provides a platform to achieve stable and good dispersion of Ni nanoparticles, but also helps improve their ability to adsorb 4-nitrophenolate ions and to capture hydrogen radicals, thereby accelerating the hydrogen transfer from metal hydride complex to 4-nitrophenol. Benefiting from the abovementioned unique features, it outperforms most Ni-based catalysts. While a 30-s re-electrodeposition of Ni can provide it extra 150 min of high catalytic activity towards the reduction of waste 4-nitrophenol to valuable 4-aminophenol, further demonstrating its outstanding reusability. The highly general methodology reported here paves the way to economically and effectively synthesize various other metal nanoparticles-loaded ZnO nanowire arrays on different conductive substrates, which not only enrich the nanowire-arrayed catalysts, but also significantly promote their practical utilizations in a wide range of environment-related fields.
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