CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Hailong Li,Weizhen He,Wei Zheng,Zequn Yang,Yingchao Hu,Wenqi Qu
The limited adsorption capacity of commercialized sorbents towards elemental mercury (Hg 0 ) remains a major challenge facing their extensive applications under the regulation of the Minamata Convention. Metal selenides were recently found to be promising alternatives to commercialized sorbents for capturing Hg 0 from industrial flue gas due to the high affinity between Hg 0 and selenide. In metal selenides, under-coordinated selenide sites play critical roles in oxidation and subsequent immobilization of Hg 0 , while there is still no simple way to increase the abundance of under-coordinated selenide in metal selenides under ambient conditions. In this work, an effective and facile precipitation pathway was proposed to prepare amorphous cobalt selenide (a-CoSe 2 ) with under-coordinated selenide enriched surface under ambient conditions. The a-CoSe 2 as synthesized achieved outstanding Hg 0 uptake capacity and adsorption rate (534.2 mg g −1 and 483.1 μg g −1 min −1 ), far surpassing those of crystalline cobalt selenide (c-CoSe 2 ) by magnitudes. The characteristic results demonstrated that the under-coordinated selenide enriched nature of a-CoSe 2 is the principal reason causing the significant performance improvement, which is fully in line with our hypothesis and purpose. This work not only proposes a potential sorbent for efficient Hg 0 sequestration from industrial flue gas but also inspires the further development of synthesis strategies for amorphous materials.
研究领域:
环境科学
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材料科学
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化学工程
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DOI
高影响因子
Energy Storage Materials
·
2017
·
IF 0
Hao Zhong,Liu Zhang Ouyang,Jian Shan Ye,Jiang Wen Liu,Hui Wang,Xiang Dong Yao,Min Zhu
The hydrolysis of NaBH 4 offers significant advantages for hydrogen storage in fuel cells, whereby suffers from the irreversibility . Thus, a simple and low cost method for NaBH 4 regeneration from its hydrolysis byproduct is crucial. Herein, we describe a single step method for NaBH 4 regeneration, which combines both hydrogen production and storage in the one step. In the process, a mixture of magnesium silicide and dihydrate sodium metaborate is reacted via ball milling under ambient conditions without the requirements of additional hydrogen sources . The hydrogen only comes from the splitting of H 2 O in the NaBO 2 ·2H 2 O that is a direct byproduct of NaBH 4 hydrolysis. The purified product demonstrates the same physicochemical properties as commercial NaBH 4 . Yields for NaBH 4 regeneration approaching 80% are achieved using this method. Mechanism study indicates that the high yield is likely to be beneficial from the formation of the Mg-O-Si-H conjugated structure. NaBH 4 regeneration using this process demonstrates a 30-fold reduction in cost over a previous study that used MgH 2 as the reduction agent.
研究领域:
化学
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材料科学
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能源存储
✓ 已验证
产品关联
DOI
RSC Advances
·
2020
·Vol. 10
·期 44
·26142-26150
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IF 3.119
Binyu Xu,Samuthirarajan Senthilkumar,Wei Zhong,Zhongquan Shen,Chunxin Lu,Xiaoming Liu
In this work, core–shell Fe3O4@Cu2O and Fe3O4@Cu2O–Cu nanomaterials for aerobic oxidation of benzylic alcohols are reported with 2,2,6,6-tetramethylpiperidine-N-oxyl (TEMPO) and N-methylimidazole (NMI) as the co-catalysts. To anchor Cu2O nanoparticles around the magnetic particles under solvothermal conditions, the magnetic material Fe3O4 was modified by grafting a layer of L-lysine (L-Lys) to introduce –NH2 groups at the surface of the magnetic particles. With amine groups as the anchor, Cu(NO3)2 was used to co-precipitate the desired Cu2O by using ethylene glycol as the reducing agent. Prolonging the reaction time would lead to over-reduced forms of the magnetic materials in the presence of copper, Fe3O4@Cu2O–Cu. The nanomaterials and its precursors were fully characterized by a variety of spectroscopic techniques. In combination with both TEMPO and NMI, these materials showed excellent catalytic activities in aerobic oxidation of benzylic alcohols under ambient conditions. For most of the benzylic alcohols, the conversion into aldehydes was nearly quantitative with aldehydes as the sole product. The materials were recyclable and robust. Up to 7 repeat runs, its activity dropped less than 10%. The over-reduced materials, Fe3O4@Cu2O–Cu, exhibited slightly better performance in durability. The magnetic properties allowed easy separation after reaction by simply applying an external magnet.
研究领域:
材料科学
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催化
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化学工程
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纳米技术
✓ 已验证
DOI
PubMed
高影响因子
Nature Communications
·
2018
·Vol. 9
·期 1
·1-8
·
IF 12.353
Qiu Weibin,Xie Xiao-Ying,Qiu Jianding,Fang Wei-Hai,Liang Ruping,Ren Xiang,Ji Xuqiang,Cui Guanwei,Asiri Abdullah M.,Cui Ganglong,Tang Bo,Sun Xuping
Conversion of naturally abundant nitrogen to ammonia is a key (bio)chemical process to sustain life and represents a major challenge in chemistry and biology. Electrochemical reduction is emerging as a sustainable strategy for artificial nitrogen fixation at ambient conditions by tackling the hydrogen- and energy-intensive operations of the Haber–Bosch process. However, it is severely challenged by nitrogen activation and requires efficient catalysts for the nitrogen reduction reaction. Here we report that a boron carbide nanosheet acts as a metal-free catalyst for high-performance electrochemical nitrogen-to-ammonia fixation at ambient conditions. The catalyst can achieve a high ammonia yield of 26.57 μg h –1 mg –1 cat. and a fairly high Faradaic efficiency of 15.95% at –0.75 V versus reversible hydrogen electrode, placing it among the most active aqueous-based nitrogen reduction reaction electrocatalysts. Notably, it also shows high electrochemical stability and excellent selectivity. The catalytic mechanism is assessed using density functional theory calculations.
研究领域:
化学
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材料科学
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电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Frontiers in Bioengineering and Biotechnology
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2023
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IF 5.7
Yang Kuan,Wei Wei,Gao Li Ting,Zhao Xin Yi,Liu Zhenqi,Li Jianhui,Li Haopeng,Miyatake Hideyuki,Ito Yoshihiro,Chen Yong Mei
The proper microenvironment is critical for the storage and transportation of embryonic stem cells (ESCs). To mimic a dynamic 3D microenvironment as it exists in vivo and consider “off-the-shelf” availability reaching the destination, we proposed an alternative approach that allows for facile storage and transportation of stem cells in the form of ESCs-dynamic hydrogel construct (CDHC) under ambient conditions. To form CDHC, mouse embryonic stem cells (mESCs) were in-situ encapsulated within a polysaccharide-based dynamic and self-biodegradable hydrogel. After storing CDHC in a sterile and hermetic environment for 3 days and then transferring to a sealed vessel with fresh medium for another 3 days, the large and compact colonies retained a 90% survival rate and pluripotency. Furthermore, after transporting and arriving at the destination, the encapsulated stem cell could be automatically released from the self-biodegradable hydrogel. After continuous cultivation of 15 generations of retrieved cells, automatically released from the CDHC, the mESCs underwent 3D encapsulation, storage, transportation, release, and continuous long-term subculture; resumed colony forming capacity and pluripotency were revealed by stem cell markers both in protein and mRNA levels. We believe that the dynamic and self-biodegradable hydrogel provides a simple, cost-effective, and valuable tool for storing and transporting “ready-to-use” CDHC under ambient conditions, facilitating “off-the-shelf” availability and widespread applications.
研究领域:
生物材料
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干细胞生物学
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组织工程
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生物技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
GREEN CHEMISTRY
·
2020
·Vol. 23
·期 3
·1382-1388
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IF 9.48
Liang Chen,Yiming Huang,Ren Zou,Jiliang Ma,Yunyi Yang,Tingzhen Li,Mingsai Li,Qi Hao,Haibo Xie,Xinwen Peng
Synthesis of D-xylonic acid, a high value chemical feedstock, from biomass chemicals through a photocatalytic process is of great significance in respect of economical and sustainable concerns, and therefore has aroused considerable attention. Herein, a TiO2/Ti3C2(TT) photocatalyst was designed for the oxidation of xylose to D-xylonic acid under ambient conditions. The photocatalyst is fabricated by in situ growth of TiO2 nano-particles on Ti3C2 nanosheets and exhibits 64.2% of D-xylonic acid yield with excellent stability. The mechanistic study indicates that the electron transfer from TiO2 to Ti3C2 significantly increases the life time of light-induced charge carriers, and hence improved photocatalytic performance.
研究领域:
材料科学
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化学工程
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可持续化学
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光催化
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2016
·
IF 3.15
Meng Tian,Xueliang Cui,Chunxu Dong,Zhengping Dong
In this study, a novel catalyst has been prepared through supporting Pd nanoparticles (NPs) on the surface of boehmite (γ-AlOOH) based hollow aluminosilicate microspheres (HAM@γ-AlOOH). The prepared Pd/HAM@γ-AlOOH catalyst has high catalytic activity for the hydrogenation of nitroarenes to their corresponding amino derivatives with high yields at ambient conditions. The high catalytic efficiency is attributed to the large pore size of the flower-like hierarchical flakes structure of HAM@γ-AlOOH, that gives Pd NPs on the support surface easy accessibility. Moreover, the Pd/HAM@γ-AlOOH catalyst can also be easily recycled at least five times without obvious decrease of catalytic activity. This work may provide a useful method for the fabrication of supported noble metal NP-based catalysts on the surface of mesoporous hierarchical structure materials with easy accessibility and superior activity.
研究领域:
催化
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材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
Nature Catalysis
·
2021
·Vol. 4
·期 7
·557-564
·
IF 41.813
Bu Jun,Liu Zhenpeng,Ma Wenxiu,Zhang Lei,Wang Tao,Zhang Hepeng,Zhang Qiuyu,Feng Xinliang,Zhang Jian
The current thermocatalytic acetylene hydrogenation process suffers from the use of excessive hydrogen and the noble metal Pd, high temperatures and overhydrogenation. Here we report an electrocatalytic semihydrogenation strategy to selectively reduce acetylene impurities to ethylene under ambient conditions. For a crude ethylene flow that contains 1 × 10 4 ppm acetylene, electrochemically deposited Cu dendrites exhibited a high specific selectivity of 97%, continuous production of a polymer-grade ethylene stream (4 ppm acetylene) at a large space velocity of 9.6 × 10 4 ml g cat –1 h –1 and excellent long-term stability. Theoretical and operando electrochemical Raman investigations revealed that the outstanding electrocatalytic acetylene semihydrogenation performance of Cu catalysts originates from its exothermic acetylene adsorption and ethylene desorption. Meanwhile, the electrocatalytic semihydrogenation strategy is universally applicable for hydrogenating other alkyne impurities to produce polymer-grade olefins, for example, propylene and 1,3-butadiene.
研究领域:
化学工程
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电化学
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催化
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2022
·
IF 5.518
Chunyang Lu,Yangqin Gao,Wei An,Chengcheng Yan,Fengshan Yu,Wenyi Lu,Chunxia Wang,Guoyong Huang
Distinct from the traditional synthesis of NiCo 2 O 4 nanoflowers from hydrothermal approach. Herein a facile gas-liquid diffusion method was exploited to prepare NiCo 2 O 4 and Fe-doped NiCo 2 O 4 nanoflower under ambient condition for oxygen evolution reaction (OER). The remarkable nanoflowers was generated by diffusing ammonia to the homogeneous solution of cobalt and nickel sulfate salt with slight amount of Fe sulfate salt to form a heterogeneous precipitation, followed by pyrolysis to afford the final product of NiCo 2 O 4 or Fe-doped NiCo 2 O 4 . The remarkable feature of NiCo 2 O 4 displays a spherical nanoflower morphology composed of lamellar structure with excellent dispersibility and greatly prompt the electron transfer and enable a high activity. By varying the ratio of Ni to Fe to 9:1, a superior OER performance with overpotential of 256 mV and Tafel slope of 69 mV·dec −1 at 10 mA·cm −2 was obtained. We attribute the superior performance to the excellent gas and ion transport channels due to the unique nanoflower structure as well as the well optimized electronic structure derived from Fe doping. Besides, we tentatively propose a detailed formation process for the formation of this nanoflower structure based on co-precipitation reaction. In conclusion, this approach offers a facile and efficient way for the preparation of high-performance ternary mixed metal oxides nanostructure which enable its large-scale production of OER catalyst.
研究领域:
材料科学
·
电化学
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纳米技术
·
催化
✓ 已验证
产品关联
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2018
·
IF 5.116
Bo Xu,Zaichun Liu,Weibin Qiu,Qian Liu,Xuping Sun,Guanwei Cui,Yuping Wu,Xiaoli Xiong
Identification of new effective and selective N 2 reduction electrocatalyst is still of critical importance for fundamental and application research. Here, we report La 2 O 3 nanoplate performing as an efficient metal oxide catalyst for electrochemical N 2 fixation to NH 3 , which exhibits excellent selectivity and stability with a high Faradaic efficiency of 4.76% and a NH 3 yield rate of 17.04 μg h −1 mg −1 cat. at −0.8 V vs. reversible hydrogen electrode (RHE) in 0.1 M Na 2 SO 4 solution under atmospheric pressure. Density functional theory (DFT) calculation results show that La atoms in La 2 O 3 act as the active sites for efficiently adsorbing N 2 . The optimal adsorption approach of N 2 molecule on the (011) face of La 2 O 3 is end-on-two configuration which is highly activated. Thus La 2 O 3 exhibits high performance for electrochemical reduction of N 2 .
研究领域:
电化学
·
催化
·
材料科学
·
理论化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Chanjuan Yang,Shoukang Xiao,Liyu Chen,Yingwei Li,Kui Shen
γ-Valerolactone (GVL) as an important high-value chemical can be readily produced through the catalytic hydrogenation of renewable levulinic acid (LA). However, high reaction temperatures (70–240 ℃) and H 2 pressures (0.5–6 MPa) are usually required to achieve full LA conversion and desired GVL yield in previous studies. Herein, we report, for the first time, the ambient-condition upgrading of LA to GVL by rationally constructing a series of metallic–acidic Ru x Pt y /MIL-101 catalysts comprising RuPt-alloyed nanoparticles (NPs) and Lewis-acid sites within a chromium-based MOF (namely MIL-101). Benefiting from the favorable synergy between Ru and Pt in their alloyed NPs and abundant Lewis-acid sites in MIL-101, the best Ru 4 Pt 1 /MIL-101 featuring an optimized Ru/Pt molar ratio of 4:1 shows a complete LA conversion with > 99.9 % yield of GVL under unprecedented ambient temperature and pressure, affording a high turnover frequency (TOF) of 1480.5h −1 , which is 15.1 and 10.1 times that of its monometallic Pt/MIL-101 (98.3 h −1 ) and Ru/MIL-101 (146.7 h −1 ) counterparts, respectively. Detailed experiments and density functional theory (DFT) calculations suggest the RuPt-alloyed effect and Lewis-acid sites in Ru 4 Pt 1 /MIL-101 can optimize the adsorption energy of 4-hydroxyvaleric acid (HPA) to remarkably boosting its catalytic performance for this reaction.
研究领域:
催化
·
绿色化学
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可再生能源
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材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
Nature Energy
·
2022
·Vol. 7
·期 11
·1042-1051
·
IF 67.439
Zhang Lili,Liu Le,Pan Ziye,Zhang Rui,Gao Zhuoyang,Wang Guangming,Huang Keke,Mu Xiaoyue,Bai Fuquan,Wang Yan,Zhang Wei,Cui Zhonghua,Li Lu
Direct non-oxidative dehydrogenation of alkanes produces useful carbon feedstocks and hydrogen fuel. However, breaking the C–H bonds in alkanes typically requires high temperature, stoichiometric oxidants or high-energy ultraviolet light; processes that operate under milder conditions are attractive but tend to have poor efficiency. Here we report Pt/black TiO 2 photocatalysts in which Pt species are close to each other but not directly bonded, exhibiting high performance for alkane dehydrogenation in visible to near-infrared light at room temperature. For cyclohexane dehydrogenation, the turnover number for H 2 production exceeded 100,000 without any deactivation over 80 reaction cycles, far beyond thermal reactions. For methane, 8.2% conversion was achieved with 65% selectivity to propane, rather than the more common ethane. We propose that methane undergoes intramolecular dehydrogenation to produce a methylene intermediate. For C2+ alkanes, fast dehydrogenation (up to 1,440 µmol g −1 h −1 ) to the corresponding olefins was realized. Distinct from isolated Pt + monomers, the collections of Pt + monomers give better photocatalytic activity and selectivity.
研究领域:
化学
·
催化
·
材料科学
·
能源
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）