ACS Applied Materials & Interfaces
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2024
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IF 8.3
You-Zhou Yang,Yun Rong,Yuan-Yuan Li,Mengmeng Ma,Dan Chen,Hang Lu,Chang Wu,Boyuan Shen,Jin-Ping Guan,Ming-Peng Zhuo
Smart materials demonstrate fascinating responses to environmental physical/chemical stimuli, including thermal, photonic, electronic, humidity, or magnetic stimuli, which have attracted intensive interest in material chemistry. However, their limited/harsh stimuli-responsive behavior or sophisticated postprocessing leads to enormous challenges for practical applications. Herein, we rationally designed and synthesized thermochromic Ni(II) organometallic [(C2H5)2NH2]2NiCl4–xBrx via a facile mechanochemical strategy, which demonstrated a reversible switch from yellow to blue color with a tunable phase-transition temperature from 75.6 to 61.7 °C. The simple electrospinning technology was applied to fabricate thermochromic Ni(II) organometallic-based nanofiber membranes for temperature monitoring. Furthermore, the organic charge-transfer cocrystal with a wide spectral absorption of 300–1950 nm and a high-efficiency photothermal conversion was combined with thermochromic Ni(II) organometallics for the desired dual-stimuli photo/thermochromism. This work supplies a new strategy for realizing multiple stimuli-responsive applications, such as thermal/light sensor displays and information storage.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Luotian Lv,Yao Liu,Yankai Huang,Tong Li,Han Feng,Yongqing Wang
Since the intensification of global environmental pollution and energy shortages, photocatalytic CO 2 reduction reaction (CO 2 RR) has emerged as a promising strategy to convert solar energy into clean chemical energy. Herein, we construct a robust and efficient heterojunction construction photocatalyst for CO 2 RR, composed of the highly reactive CeNi quantum dots (CeNi QDs) and nickel metal–organic layer (Ni-MOL) ultrathin nanosheets. This design facilitates the rapid separation of photogenerated charge carriers, as confirmed by X-ray photoelectron spectroscopy (XPS), photoluminescence spectroscopy (PL) and other characterizations. Mechanistic studies with in situ diffuse reflectance Fourier transform infrared spectroscopy (in situ DRIFTS) and the d-band center calculation indicate that the propensity of photocatalyst for CO 2 absorption and CO desorption, leading to high performance and selectivity. The optimized loading amount of CeNi quantum dots and modified structure result in a CO yield of 30.53 mmol·g −1 within 6 h under irradiation. This work not only paves a new and convenient way for developing high-activity quantum dot materials for CO 2 RR but also exploits novel avenues to fabricate more heterojunction composites for solar energy conversion.
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高影响因子
CATALYSIS TODAY
·
2024
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IF 5.2
Yanan Jiang,Huayu Sun,Yuzhen Fang,Cuijuan Zhang,Yuan Liu
The sintering issue of Ni nanoparticles seriously limits the practical application of the Ni-based catalysts for CO 2 methanation. This work demonstrates that the La- and Ce- dual-promoted Ni/ZrO 2 shows better durability at 600 ºC and 60000 mL g cat −1 h −1 over 200 h compared with the La- or Ce- single-promoted. The composition and microstructure characterization indicates that the dispersion and sintering resistance of Ni nanoparticles is enhanced with the dual-promoted catalysts. Both depth profile of X-ray photoelectron spectroscopy and density functional theory calculation show that in the La- and Ce- dual-promoted Ni/ZrO 2 , the reduced dissolution of Ce into ZrO 2 lattice and the spread of La on ZrO 2 surface by forming a La 2 O 3 -CeO 2 solid solution improves the dispersion and stability of Ni nanoparticles. This work provides a facile strategy to mitigate the sintering of Ni nanoparticles and thus improve the stability of Ni-based catalysts for CO 2 methanation.
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APPLIED CATALYSIS A-GENERAL
·
2024
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IF 4.7
Xiaofei Li,Lili Geng,Haifeng Shi,Songshou Ye,Ley Boon Sim,Jinbao Zheng,Nuowei Zhang,Binghui Chen
In this study, we utilized a sol-gel method to prepare Ni-HPW/SiO 2 catalysts with varying citric acid (CA):Ni molar ratios ranging from 0 to 5.0. The catalysts demonstrated different levels of activity in the hydrogenation of ethylbenzene , which correlated to their respective CA:Ni ratios. Introducing citric acid in the preparation process of nickel-based catalysts yielded mesopore formation and reduced NiO particle size, producing a more uniform NiO dispersion on SiO 2 , which was confirmed by BET, XRD, and TEM analyses. The results of H 2 -TPR, H 2 -TPD, NH 3 -TPD, and Py-IR analyses suggested that the addition of citric acid augmented the interaction between phosphotungstic acid (HPW), Ni species, and SiO 2 . Citric acid improved Ni species and HPW dispersion, fostering increased HPW-Ni species formation. This, in turn, generated additional electron-deficient Ni ions , stemming from semi-reduced HPW-Ni species, which acted as Lewis acid sites, enhancing Ni + species effectiveness in activating aromatic rings. The better-dispersed, non-HPW-bound NiO, which, upon complete reduction to Ni, led to a substantial rise in H 2 bond cleavage, thereby facilitating more hydrogen spillover. Overall, the infusion of citric acid into fabricating Ni-HPW/SiO 2 catalysts sparked a significant surge in their aromatic hydrogenation ability.
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Molecular Catalysis
·
2024
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IF 3.9
Guili Luan,Guihua Yang,Hongyu Wang,Jiaxuan Li,Haojie Sun,Mengyao Sun,Changfei Shi,Shitao Yu,Ji-Jun Zou,Genkuo Nie
(Alkyl-)cyclohexane diols are of high value as industrial reagents and resources, but current producing methods are still unsustainable. Herein, a new method of producing (alkyl-)cyclohexane diols using lignin derived phenols with yield as high as 91.2 % by selective hydrogenolysis is firstly achieved over Nb 2 O 5 and Ni/MCM-41. The hydrogenolysis is completed by designing two-step reactions compositing of selective crack of C(sp 3 )-O bond and selective hydrogenation of benzene ring of lignin derived phenols to achieve a high selectivity. Nb 2 O 5 demonstrates superior activity and long-life time in C(sp 3 )-O bond cleavage compared to commercial solid acids. The robust catalytic performance was thoroughly analyzed through detailed characterization and attributed to the abundant oxygen vacancies produced, which lead more strong L acids and adsorb the methoxy group in lignin derived phenols and at the same time interact with the acid sites to facilitate the cleavage of the C(sp 3 )-O bond. The consequent selective hydrogenation of benzene ring is completed by Ni/MCM-41 easily. More lignin derived phenols are explored in this reaction with (alkyl-)cyclohexane diols universally synthesized. This work provides a new application of lignin derived phenols to synthesize value-added chemicals and makes contribution to sustainable development by biorefineries.
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Molecular Catalysis
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2025
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IF 4.9
Zhen Zhang,Minghui Yu,Meiqing Shen,Wei Li,Gurong Shen
Ni-based catalysts, as non-noble metal alternatives, are widely regarded for their potential in ammonia decomposition for hydrogen production. However, their performance at low temperatures is suboptimal, necessitating the addition of promoters and a clear understanding of their mechanisms to enhance catalytic activity. In this study, we have successfully improved the low-temperature ammonia decomposition performance of Ni/CeO 2 by incorporating alkaline earth metals and conducted a comprehensive analysis of the underlying structural and electronic effects. The findings reveal that alkaline earth metals can enhance the basicity of the catalyst and increase electron density around the active metal sites, thereby facilitating the rate-determining step of recombination and desorption of N atom. Moreover, the presence of alkaline earth metals disrupts hydrogen adsorption stability on the catalysts, effectively mitigating the impact of hydrogen inhibition. Based on systematic kinetic experiments, a kinetic model was developed that accurately captures the hydrogen inhibition effect for Ni/CeO 2 catalysts. The insights into the promotional mechanisms of alkaline earth metals offer theoretical guidance for the development of highly active and cost-effective catalysts for ammonia decomposition.
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APPLIED SURFACE SCIENCE
·
2024
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IF 6.3
Qiang Fang,Lu Hao,Tao Zhao,Jiahui Li,Genyan Hao,Guang Liu,Dazhong Zhong,Jinping Li,Qiang Zhao
The electrocatalytic production of 2,5-furandicarboxylic acid (FDCA) via the 5-hydroxymethylfurfural oxidation reaction (HMFOR) is an effective and more suitable alternative to the oxygen evolution reaction (OER) in electrocatalytic water splitting. High-valence Ni(III) is critical for the HMFOR, but the formation is greatly limited by the difficult in situ self-oxidation. In this study, the pre-oxidization-derived amorphous NiO x H y nanosheet presents more accessible Ni(III) for efficient HMFOR. In addition, NiO x H y /NF exhibits a low onset potential of 1.35 V, a high FDCA yield of 98.5 %, and a high Faradaic efficiency of 98.3 % for the HMFOR in 0.1 M KOH with 10 mM HMF. In situ Raman spectroscopy results indicate that Ni(III)OOH is an active intermediate in the electrochemical HMFOR. This work provides a strategy for promoting the formation of high-valence Ni(III) and boosting biomass oxidation.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2020
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IF 4.939
Zhonghui Zhang,Changlei Qin,Zhiliang Ou,Jingyu Ran
H 2 S is a kind of common impurity produced during the gasification of biomass, and it will poison the catalysts used in biomass tar steam reforming , leading to a rapid degradation on the catalytic performance. The purpose of this work is to investigate the characteristics of biomass tar steam reforming using Ni/perovskite catalysts with the presence of H 2 S. Results show that H 2 S could significantly reduce catalytic activity due to the adsorption of sulfur on Ni surface , and Ni/perovskite catalysts are less susceptible to this poisoning in comparison to the Ni-catalyst loaded on γ-Al 2 O 3 . To understand the mechanism, fresh and spent catalysts were characterized using various techniques of XRD , SEM-EDS, XPS and TPO . It is proved that the lattice oxygen in perovskite could transform into surface species, inhibit the adsorption of sulfur and thus benefit to the reactivity of catalysts during biomass tar steam reforming.
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ACS Catalysis
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2022
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IF 13.7
Xiangze Du,Xiaomei Lei,Linyuan Zhou,Yong Peng,Yan Zeng,Huiru Yang,Dan Li,Changwei Hu,Hermenegildo Garcia
In the context of the preparation of liquid fuels derived from biomass with zero CO2 footprint, fatty acids appear as suitable feedstocks. However, reduction of carboxylic acid groups usually requires harsh reaction conditions and the development of efficient solid catalysts. Herein, bimetallic Ni–Mo nitrides have been obtained by a procedure not involving nitridation of the corresponding oxide, but reductive decomposition of the tris(ethylenediamine)nickel molybdate at temperatures between 550 and 700 °C. Successful formation of the Ni3Mo3N nitride is confirmed by X-ray diffraction. Ni3Mo3N samples are found to be efficient catalysts for the hydrodeoxygenation of palmitic acid to C15/C16 alkanes with a combined selectivity over 90 and 100% palmitic acid conversion and higher activity than analogous Ni–Mo nitrides obtained by NH3 nitridation of NiMoO4. Ni3Mo3N is found recyclable with only a slight decay in the catalytic activity upon consecutive reuses attributable to the neutralization of acid sites. The present results show an opportunity that bimetallic nitrides offer as robust advanced solid catalysts for reactions of biomass conversion requiring harsh conditions.
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SURFACE & COATINGS TECHNOLOGY
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2022
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IF 4.865
Hongjie Li,Yi He,Pingya Luo,Huilian Zhou,Bo Liu,Yahui He,Ruxia Song,Zhifei Zhang,Yi Fan
In this study, a novel superhydrophobic composite coating is prepared by a two-step method. Firstly, the Ni-based deposition coating is fabricated via composite electrodeposition with WS 2 granules worked as dispersed phase particles, and the roughness of deposit coating can be adjusted by changing the added amount of sulfide in the bath. The prepared Ni-WS 2 deposit exhibits sufficiently high roughness and suitable micro-nano morphology. Then, hexadecyltrimethoxysilane (HDTMS) is used to modify the deposition coating with low surface energy to obtain silanol-modified Ni-WS 2 coating with superhydrophobic properties. The superhydrophobic behavior of the composite coating conforms to the Cassie-Baxter model, with low adhesion to aqueous solutions. When the addition amount of WS 2 particles in the plating solution during the electrodeposition process is 5 g·L −1 , the prepared composite coating has the excellent superhydrophobic properties. The water contact angle of the composite coating is 154.7° ± 2 and the sliding angle can reach 6°. And the superhydrophobic composite coating exhibits excellent corrosion resistance .
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Zongze Lv,Jiaqi Ruan,Weifeng Tu,Xun Hu,Donglin He,Xin Huang,Changlei Qin
Integrated carbon capture and utilization by methanation (ICCU-methanation) is an emerging concept in reducing CO 2 emissions and storing H 2 simultaneously. One key of the technology is the development of dual functional materials (DFMs) that can efficiently capture CO 2 and then catalyze it. Herein, we propose the construction of DFM using Li 4 SiO 4 with superior CO 2 adsorption/desorption features as sorbent and catalyst carrier, CeO 2 as catalyst promoter and isolator, and Ni as catalytic metal, and comprehensively evaluate its characteristics and performance in ICCU-methanation. Results show that the DFM developed possess a high and stable CO 2 capacity of 5.4 mmol·g DFM -1 , 96 % CO 2 conversion and 96 % CH 4 selectivity under both the ideal CO 2 capturing atmosphere and the realistic flue gas containing 10 vol% steam and 8 vol% O 2 . Moreover, rapid CO 2 dissociation from the DFM is observed at a temperature lower to 560 °C due to the reaction of H* dissociated by catalyst with carbonate to form formate, which further decomposes to release CO.
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ACS Applied Materials & Interfaces
·
2016
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IF 7.145
Naijian Ge,Donghui Wang,Feng Peng,Jinhua Li,Yuqin Qiao,Xuanyong Liu
Drug-eluting stents (DESs) are widely used in the palliative treatment of many kinds of cancers. However, the covered polymers used in DESs are usually associated with stent migration and acute cholecystitis. Therefore, developing noncovered drug-loading layers on metal stents is of great importance. In this work, Ni–Ti layered double hydroxide (Ni–Ti LDH) films were prepared on the surface of nitinol via hydrothermal treatment, and the LDH films were further modified by poly(styrenesulfonate) (PSS). The anticancer drug doxorubicin could be effectively loaded onto the modified films, and drug release could be smartly controlled by the pH. Besides, the drug absorption amounts of cancer cells cultured on the films could be effectively improved. These results indicate that the PSS-modified LDH film may become a promising drug-loading platform that can be used in the design of DESs.
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