CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Fei Fan,Xiaodi Zhu,Jiacan Kang,Zhenyu Song,Jianwei Liu,Hailong Wang,Anning Zhou,Houxiang Sun,Zhiping Chen,Wenwu Zhou
Developing high-performance non-precious metal catalysts for liquid organic hydrogen storage is crucial for advancing hydrogen energy technologies. Herein, we proposed a strategy in which doped Ge promoters optimized electron environments of nGeNi active phase loaded on titanium-aluminum composite oxide support with highly ordered 2D hexagonal mesopores (nGeNi/TA, n = 0, 0.5, 1, and 2 wt%), successfully establishing electron-rich active phase with high matching to HOMO orbital of N-Ethylcarbazole (NEC) molecule. Meanwhile, both d-band center of active phase and electron densities of its conduction band were effectively adjusted. These improvements not only retained ability of nGeNi active phase to activate NEC and its intermediates, but also suitably weakened strong π-d interaction with their aromatic rings. Consequently, adsorption energy of each intermediate species was almost close to average energy of hydrogenation conversion stages, thereby decreasing desorption energy of complete hydrogenation product (12H). Compared with 0GeNi/TA catalyst, NEC conversion rate on the best 1GeNi/TA catalyst at low temperature (220℃) greatly increased by approximately 118 %, and 12H selectivity and its yield sharply improved by approximately 112 % and 132 %, respectively. Moreover, excessive accumulations of intermediate species were also effectively mitigated.
研究领域:
催化化学
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能源材料
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纳米材料
·
表面科学
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氢能源技术
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MATERIALS CHEMISTRY
·
2012
·Vol. 22
·期 33
·16872-16879
·
IF 5.968
Zai-lin Gong,Dong-yan Tang,Yu-di Guo
This article reports on the fabrication of hybrid titanium dioxide (TiO2) nanoparticles grafted with thermoresponsive poly(N-isopropylacrylamide) (PNIPAM) and their self-flocculation effect caused by the thermal phase transition and entanglement behavior of PNIPAM. Surface-initiated atom transfer radical polymerization (ATRP) of N-isopropylacrylamide (NIPAM) was conducted rapidly (within a few minutes) in aqueous solution at ambient temperature by using CuBr/N,N,N′,N′′,N′′-pentamethyldiethylenetriamine (PMDETA) as the catalysts and started from the surface of TiO2 nanoparticles derivatized with ATRP initiators. Without purifying the inhibitor, the grafted PNIPAM gives low molecular weights (Mn < 3000) and a narrow molecular weight distribution (PDI < 1.1) determined by GPC detection, which gives the hybrid TiO2–PNIPAM both a self-flocculation effect with rapid response to temperature, and a temperature-controlled switching effect of the degradation of Rhodamine B in solution. Moreover, the hybrid TiO2–PNIPAM exhibits a particular dispersion effect at ambient temperature in aqueous solution caused by the hydrophilicity and the entanglement interaction of the grafted PNIPAM. These effects for hybrid TiO2–PNIPAM provide a new way to re-use TiO2 nanoparticles for pollutant degradation systems and to avoid secondary pollution effectively due to the thermal phase transition and entanglement behavior.
研究领域:
材料科学
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环境科学
·
高分子化学
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DOI
高影响因子
WORLD JOURNAL OF MICROBIOLOGY & BIOTECHNOLOGY
·
2017
·Vol. 33
·期 2
·1-9
·
IF 1.658
Zhang Jian-Fen,Chen Wei-Qing,Chen Hong
In this study, we report the cloning and expression of a functional glucoside 3-dehydrogenase (G3DH) gene from Sphingobacterium faecium ZJF-D6. This gene is 1686 bp in length and encodes a peptide of 562 amino acids. The G3DH gene was successfully expressed in E. coli , and the recombinant enzyme could oxidize glucosides, galactosides and analogues at C-3 position. The sequence and multiple alignment analysis showed that the enzyme has highest identity with G3DHs from Paraglaciecola polaris LMG 21857, Aliiglaciecola lipolytica E3 and Halomonas sp. alpha-15. The recombinant G3DH was purified on Ni–NTA column and exhibited the highest activity at pH 7.6 and 30 °C. It was sensitive to acid and alkali, and showed well thermostability. The SfG3DH could oxidize a wild range of sugars. When recombinant E. coli BL21 cells were used as catalyst, a high rate of conversion to N- p -nitrophenyl-3-ketovalidamine was achieved, and no p -nitroaniline was detected. This process offers a promising approach to fulfill substrate of 3-ketovalidoxylamine A C–N lyase production.
研究领域:
微生物学
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生物化学
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酶学
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生物催化
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DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Junke Li,Mei Li,Youji Li,Xin Guo,Zhiliang Jin
The exploration of multiple composite with heterojunction structures to replace single catalysts with insufficient capacity is significant for the photocatalytic evolution of high-yield hydrogen. In this case, the Mo 2 S 3 /Bi 2 O 2 CO 3 composite with a unique n-n heterojunction and two-dimensional (2D) spatial structure was successfully prepared for the first time using the hydrothermal-physical mixture method. The percentage of Bi 2 O 2 CO 3 in the composite can be easily adjusted by changing the amount of Bi 2 O 2 CO 3 introduced into the physical mixing process. With a mass percentage of Bi 2 O 2 CO 3 attained 3% to Mo 2 S 3 , the composite Mo 2 S 3 /Bi 2 O 2 CO 3 with n-n heterojunction exhibited the highest photocatalytic effect among all as-prepared samples, with a photocatalytic effect 5 times higher than pure Mo 2 S 3 . The presence of Bi 2 O 2 CO 3 and the synergistic interactions of n-n heterojunction significantly reduced the dispersity of short-rod shaped Mo 2 S 3 , as well as the recombination of photogenerated charge carriers. As a result, electron circulation was improved, and photocatalytic hydrogen evolution activity under visible light was improved. In addition to improving the photocatalytic hydrogen evolution effect, the composite Mo 2 S 3 /Bi 2 O 2 CO 3 has been found to have excellent stability, which is a noteworthy feature. A series of characterization results and semiconductor energy band structure were used to investigate the possible photocatalytic hydrogen evolution mechanism in the Eosin-Y (EY) sensitized Mo 2 S 3 /Bi 2 O 2 CO 3 system.
研究领域:
材料科学
·
能源科学
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DOI
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2024
·
IF 3.9
Jialu Wei,Jingyu Wang,Wei Zhang,Yuezhen Mao,Chunwen Sun
Graphical A ZAB with Co–N–C–PBMCRO cathodic catalyst achieves a remarkable cycling stability for 788 h. The perovskite Pr 0.5 Ba 0.5 Mn 0.8 Co 0.1 Ru 0.1 O 2.5+δ (PBMCRO) composite was constructed by in situ exsolved CoRu nanoparticles and Co–N–C with more exposing active sites. A conductive pathway for oxygen ions and electrons was built, thereby enhancing the electrochemical bifunctional properties. This rational design strategy shows great potential for facilitating synthesis of perovskite based catalysts for energy conversion and storage applications. Bifunctional catalysts for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) are essential components of rechargeable zinc-air batteries. In this study, we synthesized a Pr 0.5 Ba 0.5 Mn 0.8 Co 0.1 Ru 0.1 O 2.5+δ (PBMCRO) perovskite composite with in situ exsolved CoRu nanoparticles and Co–N–C, functioning as an efficient bifunctional electrocatalyst for zinc-air batteries. The in situ exsolution of CoRu nanoparticles from the perovskite oxide was facilitated by the reducing action of 2-methylimidazole (2-MIM). Concurrently, Co–N–C was used to decorate PBMCRO, forming a novel bifunctional composite electrode of Co–N–C–PBMCRO. The incorporation of CoRu nanoparticles introduces a significant number of electrochemically active oxygen vacancies in the perovskite matrix, enhancing ORR and OER performance. Additionally, the Co–N–C synergistically improves electrochemical activity while preserving the structural stability of the perovskite oxide. The prepared Co–N–C–PBMCRO catalyst demonstrates significantly enhanced bifunctional performance compared to the undecorated pristine perovskite Pr 0.5 Ba 0.5 MnO 3−δ (PBMO). The zinc-air battery with Co–N–C–PBMCRO catalyst achieve a peak power density of approximately 90 mW/cm 2 and exhibit remarkable cycling stability for 788 h. This study presents a novel and effective strategy to enhance the catalytic performance of perovskite-based air electrodes for rechargeable metal-air batteries.
研究领域:
材料科学
·
电化学
·
能源存储与转换
✓ 已验证
DOI
高影响因子
POLYMER
·
2019
·
IF 3.771
Qingchi Ma,Li Han,Hongwei Ma,Pibo Liu,Heyu Shen,Lincan Yang,Chao Li,Xinyu Hao,Yang Li
Alternating copolymers consisting of a kind of mild electron-withdrawing 1,1-diphenylethylene (DPE) derivative and di-olefins, such as 1,1-bis(4-dimethylsilylphenyl)ethylene (DPE-2SiH) and isoprene (Ip), were successfully synthesized via anionic copolymerization using N,N,N′,N′ -tetramethylethylenediamine (TMEDA) as the modifier and benzene as the solvent. Two mild electron-withdrawing groups (binary -SiH) existed in this system. Therefore, the reaction activity of DPE-2SiH was higher than that of dimethyl-[4(1-phenylvinyl)phenyl]silane (DPE-SiH), and DPE-2SiH was expected to be an appropriate co-monomer for polymerization with dienes. The addition of TMEDA was found to not only control the resulting sequence but also regulate the contents of cis- and trans- structures in the Ip units. To further explore the mechanism of polymerizing DPE-2SiH and isoprene with and without the use of the TMEDA additive, the target samples were carefully characterized by SEC, 1 H NMR and in situ 1 H NMR. By examining the results, the apparent rate constants of DPE-2SiH and Ip without TMEDA were 1.19 × 10 −3 min −1 and 1.29 × 10 −2 min −1 , respectively, while those of DPE-2SiH and Ip with TMEDA were 4.47 × 10 −5 min −1 and 3.05 × 10 −5 min −1 , respectively. The reactivity ratios r Ip of isoprene with and without TMEDA were also calculated by the least square method and found to be 0.65 and 4.21, respectively, which illustrates the mechanisms of the copolymerization of DPE-2SiH and isoprene. By investigating the mechanism of the copolymerization process, the sequence can be controlled the alternating copolymerization, which can be facilely realized in a nonpolar solvent through the use of TMEDA. The alternating copolymers using this method have great significance both to regulation method of the microstructure of isoprene units and to the industrial production of functionalized materials. Then the alternating copolymers of DPE-2SiH and Ip were also applied to synthesize centipede-shaped grafted poly(isoprene)s (PIps). For the existence of bilateral -SiH groups in the chain, hydrosilylation of -SiH and alkynyl groups was performed at room temperature to avoid the unexpected reaction of the -SiH and alkenyl groups from the PIp branches.
研究领域:
高分子化学
·
材料科学
✓ 已验证
DOI
高影响因子
TALANTA
·
2020
·
IF 5.339
Qiurong Luo,Zhirong Zhong,Yunchao Zheng,Die Gao,Zhining Xia,Lujun Wang
The poly( N -isopropylacrylamide) (NIPAAm) was first polymerized onto the surface of graphene quantum dots (GQDs) functionalized silica as packing materials via reversible addition-fragmentation chain transfer (RAFT) polymerization reaction, which can expand the interaction modes between stationary phase and analytes. A series of characteristic methods were selected to estimate the chemical bonding results of silica, involving Fourier transform infrared spectroscopy (FT-IR), elemental analysis (EA), thermogravimetric analysis (TGA) and scanning electron microscope (SEM). The prepared column can exhibit reversed-phase and hydrophilic interaction modes, which were demonstrated by the retention of eight kinds of target analytes with different Log P values. The column was then applied to separate banlangen granules and further verified by HPLC tandem time-of-flight mass spectrometry (HPLC/QTOF-MS). In conclusion, Sil-GQDs-PNIPAAm stationary phase improved the analysis range and performance of traditional phases, exhibiting flexible selectivity and application prospect for both hydrophobic and hydrophilic analytes.
研究领域:
材料科学
·
分析化学
·
生物医学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Lixi Chen,Ying Wang,Yaoshuang Wan,Yimin Cai,Yanqi Xiong,Zhenwang Fan,Steven D. Conradson,Haiying Fu,Lihua Yuan,Wen Feng
Pillararenes, a rising star in macrocyclic chemistry, are recognized as promising organic materials for metal ion separation. Herein, three novel pillar[5]arenes ( 1a-c ) appended with N,N -dimethyldithiocarbamoyl groups were designed for highly efficient extraction of aqueous mercury. This work represents the first case of using pillararene-based materials for organic mercury removal, and rather low Hg(II) residue (3.45 ppb) was found in the extraction raffinate of mercury spiked river water after being treated with the as-prepared extractants, which is a rare example of solvent extraction systems that meet the waste water discharge standard (<5 ppb). The extraction performance of the extractant materials was evaluated under different acidities, equilibrium time and sodium nitrate concentrations. High extraction efficiency (>99%) and selectivity (SF Hg/M > 690) were achieved under the optimum condition, and the near quantitative stripping after two contacts enable regeneration of the ligands as well as mercury recovery. The stoichiometric ratio between ligands and Hg 2+ was ascertained to be 1:1 from the slope analysis method and mass spectroscopy. Investigation of the extracted species by NMR, IR, EXAFS techniques and DFT simulation reveals that the C=S moieties of the ligands play a crucial role in metal complexation. It is noted that the as-prepared extractants show excellent recovery and removal ability towards mercury using simulated samples. After extraction by 1c , the total Hg(II) in spiked river samples was reduced to lower than 5 ppb, the maximum tolerable concentration set by China for industrial waste water. This study demonstrates the potential application of N,N -dimethyldithiocarbamoyl modified pillararenes as functional materials for aquatic mercury remediation.
研究领域:
环境科学
·
材料化学
✓ 已验证
DOI
高影响因子
GREEN CHEMISTRY
·
2011
·Vol. 13
·期 5
·1352-1361
·
IF 5.472
Hengquan Yang,Yunwei Wang,Yong Qin,Yanzhu Chong,Qiaozhen Yang,Guang Li,Li Zhang,Wei Li
Based on a reverse micelle strategy, we successfully synthesized new magnetic silica nanoparticles functionalized with a bulky N-heterocyclic carbene (N,N′-bis(2,6-diisopropylphenyl)imidazol-2-ylidene, denoted as IPr) precursor through the co-condensation of IPr-bridged organosilane and tetraalkoxysilane in a one-pot reaction. TEM and SEM investigations revealed that the particle sizes of the synthesized materials were uniformly distributed in the range 15–30 nm, and could be tuned by varying the amount of siliceous precursors. FT-IR and XPS characterizations showed that the IPr ligand was successfully incorporated onto magnetic silica nanoparticles. Such materials show good coordination capability toward Pd(acac)2 (acac = acetylacetonate), leading to a higher loading in comparison with magnetic silica nanoparticles (without functionalization). This Pd-loaded material is active toward the Suzuki–Miyaura couplings of challenging aryl chlorides under relatively mild conditions (at 80 °C). An 81% yield for biphenyl was achieved in the presence of 0.32 mol% of Pd within 8 h, using iso-propyl alcohol as a solvent and KOtBu as a base. The activity of the functionalized nanoparticles is much higher than that of mesoporous silica-based catalysts, as well as a commercial Pd/C catalyst. This catalyst can be easily isolated by using a magnetic field and directly used in the next reaction cycle without significant loss of its activity.
研究领域:
纳米催化
·
有机合成方法学
·
材料化学
·
绿色化学
·
均相/非均相催化
✓ 已验证
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2019
·
IF 3.375
Tongtong Shen,Hao Peng,Xiang Ling
In this study, the phase diagrams for the binary systems of n-C11H24–n-C14H30, n-C12H26–n-C13H28, n-C12H26–n-C14H30, and n-C13H28–n-C15H32 were experimentally investigated to employ potential phase change materials (PCMs) for cryogenic applications. Besides, the phase diagrams were theoretically obtained on the basis of the ideal solubility and UNIFAC models, and the UNIQUAC, Wilson, and NRTL models were applied to build correlations between experimental and predicting values. The results show that the compositions of the eutectic points appear at 10 wt % C14 for the C11–C14 system, 17.8 wt % C13 for the C12–C13 system, 18 wt % C14 for the C12–C14 system, and 10 wt % C15 for the C13–C15 system with eutectic temperatures of 246.85, 257.75, 260.45, and 265.55 K, respectively. Moreover, the melting temperatures calculated using the theoretical models are in good agreement with the experimental results. The average relative deviations for the C11–C14 system and C13–C15 systems are merely 0.3814% and 0.3220%, respectively, by using the NRTL model. Simultaneously, the minimum relative deviations for the C12–C13 and C12–C14 binary systems are 0.3649% for the ideal solubility model and 0.4856% for the UNIFAC model. Finally, upon comparing the predicted results of the studied binary systems using the results of the five models, we find that the UNIFAC model provides the most accurate results for the melting temperatures.
研究领域:
热力学
·
储能技术
·
化学工程
·
相变材料
·
低温工程
✓ 已验证
DOI
高影响因子
Sustainable Energy & Fuels
·
2024
·Vol. 8
·期 9
·1983-1991
·
IF 5
Xianli Wu,Ting Zhou,Guosheng Han,Shuling Liu,Mengmeng Cao,Shuqi Li,Jiawen Wang,Yanyan Liu,Jianchun Jiang,Yongfeng Wang,Baojun Li
Low-cost and efficient electrocatalysts for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) are vital for the applications of flexible rechargeable zinc–air batteries (ZABs). Herein, three-dimensional (3D) porous N-doped Paulownia-derived carbon modified with FeP nanoparticles (FeP@NPW) was used as a bifunctional catalyst for flexible rechargeable ZABs. The FeP@NPW electrocatalyst exhibits a first-class bifunctional activity for the ORR and OER. The descriptor ΔE between the half-wave potential of the ORR and the potential of the OER at 10 mA cm−2 was 0.65 V. The flexible rechargeable ZABs have a high open circuit voltage of 1.43 V and superior cycle stability (over 70 h). Coupling 3D hierarchical pores of NPW and FeP facilitates charge exchange, mass transfer, and electron transportation. A high concentration of FeP sites was available during the reaction because of the large specific surface area (798 m2 g−1) of FeP@NPW. The synergistic effects between N-doped biomass-derived carbon and FeP nanoparticles improve the catalytic activity towards the ORR and OER. This work paves the way for the conversion of abundant biomass into high-value engineering products and the application of transition metals in the energy conversion and storage field.
研究领域:
材料科学
·
电化学
·
能源存储与转换
·
催化
✓ 已验证
DOI
高影响因子
ACS Omega
·
2018
·
IF 0
Changfen Bi,Yulu Liang,Lijin Shen,Shanshan Tian,Kai Zhang,Yiliang Li,Xiwen He,Langxing Chen,Yukui Zhang
Efficient enrichment glycoproteins/glycopeptides from complex biological solutions are very important in the biomedical sciences, in particular biomarker research. In this work, the high hydrophilic polyethylenimine conjugated polymaltose polymer brushes functionalized magnetic Fe3O4 nanoparticles (NPs) denoted as Fe3O4–PEI–pMaltose were designed and synthesized via a simple two-step modification. The obtained superhydrophilic Fe3O4–PEI–pMaltose NPs displayed outstanding advantages in the enrichment of N-linked glycopeptides, including high selectivity (1:100, mass ratios of HRP and bovine serum albumin (BSA) digest), low detection limit (10 fmol), large binding capacity (200 mg/g), and high enrichment recovery (above 85%). The above-mentioned excellent performance of novel Fe3O4–PEI–pMaltose NPs was attributed to graft of maltose polymer brushes and efficient assembly strategy. Moreover, Fe3O4–PEI–pMaltose NPs were further utilized to selectively enrich glycopeptides from human renal mesangial cell (HRMC, 200 μg) tryptic digest, and 449 N-linked glycopeptides, representing 323 different glycoproteins and 476 glycosylation sites, were identified. It was expected that the as-synthesized Fe3O4–PEI–pMaltose NPs, possessing excellent performance (high binding capacity, good selectivity, low detection limit, high enrichment recovery, and easy magnetic separation) coupled to a facile preparation procedure, have a huge potential in N-glycosylation proteome analysis of complex biological samples.
研究领域:
生物医学科学
·
蛋白质组学
·
纳米技术
·
分析化学
✓ 已验证
DOI
PubMed
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