APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Dejian Zhao,Zhihong Wang,Shuaishuai Lyu,Yunhao Liu,Shaohui Xiong,Yingtian Zhang,Yu Pan,Qingpeng Cheng,Xingang Li
Non-classical Fischer–Tropsch to olefins (FTO) is a crucial yet highly complex industrial reaction that enables the direct conversion of syngas, derived from renewable feedstocks such as biomass, municipal solid waste, or captured CO 2 , into long-chain olefins (C 5+ = ) via a carbide mechanism. Here, we systemically investigate mechanisms and performance of Na-modified Ru/TiO 2 catalysts in non-classical FTO, and experimentally discover a new CO insertion pathway. Our findings show that Na modification alters the adsorption and activation behaviors of CO, H 2 and intermediates, eventually manipulating reaction mechanisms. The Ru/TiO 2 catalyst with less Na exhibits high CO dissociation and C-C coupling abilities but a poor dehydrogenation ability, which mainly obeys the carbide mechanism, benefiting to produce C 5+ alkanes, rather than olefins. However, excessive addition of Na would primarily make the Ru/TiO 2 catalyst alternately follow the CO insertion mechanism, preferring to produce short olefines (C 2-4 = ) because of the poor C-C coupling ability. After rational coordination of the two pathways through regulating the Na loadings, the 0.5NaRu/TiO 2 catalyst robustly exhibits ultra-high C 5+ = selectivity (80.9%) and impressive C 5+ = space time yield (1.68 × 10 -2 mol CO g cat -1 h -1 ) at 260 °C, without deactivation for over 100 h. These findings not only provide fundamental insights into the underlying mechanisms for long-chain olefin synthesis, but also offer theoretical guidance for developing advanced catalysts for industrial applications.
研究领域:
催化化学
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能源化学
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材料科学
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产品关联
DOI
高影响因子
Journal of Physical Chemistry C
·
2021
·
IF 4.126
Fuyong Zhang,Wei Zhou,Xuewei Xiong,Yuhao Wang,Kang Cheng,Jincan Kang,Qinghong Zhang,Ye Wang
Catalytic transformation of CO2 into chemicals in large demand such as ethanol has attracted much research attention under the background of establishing carbon-neutral societies. Supported Rh catalysts are promising candidates for the hydrogenation of CO2 to ethanol but suffer from low ethanol productivity and poor catalyst stability. Here, we report that zeolite silicalite-1 embedded Na-promoted Rh nanoparticles (Na-Rh@S-1) demonstrate high productivity and stability for CO2 hydrogenation to ethanol. The ethanol selectivity of 24% was attained at a CO2 conversion of 10%, and the space-time yield of ethanol reached 72 mmol gRh–1 h–1, which outperformed most of the Rh-based catalysts reported to date. While a reference catalyst prepared by impregnation underwent deactivation, the Na-Rh@S-1 catalyst was stable for at least for 100 h owing to the confinement effect. The Na+ modifier played crucial roles in enhancing the CO2 conversion and ethanol selectivity by suppressing methane formation. The characterizations suggest that the presence of Na+ enables the coexistence of Rh0 and Rh+ and enhances CO2 adsorption, thus boosting ethanol formation. A comparative study between CO and CO2 hydrogenation reveals that the Na-Rh@S-1 catalyst is significantly more active and selective toward CO2 hydrogenation to ethanol.
研究领域:
催化化学
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环境科学
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材料科学
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产品关联
DOI
高影响因子
CATALYSIS TODAY
·
2021
·
IF 6.766
Haripal Singh Malhi,Chao Sun,Zhengzhou Zhang,Yangyang liu,Wenqi Liu,Pengchao Ren,Weifeng Tu,Yi-Fan Han
This study unravels the effects of Na decoration and/or ZnO addition on the structures of Fe based catalysts, and the reaction pathways and the rate dependencies on both the composition of reactants and reaction temperature for CO 2 hydrogenation to olefins, using kinetics and structure characterization by Raman spectroscopy, X-ray diffraction, and temperature-programmed CO reduction techniques. CO 2 hydrogenation over Fe based catalysts occurs as a combination of the primary reverse water-gas-shift reaction to form CO and the subsequent CO hydrogenations to produce olefins and paraffins. Adding ZnO into Fe catalysts enhanced the rates of CO 2 hydrogenation to all carbon containing products because ZnO facilitated the generation of iron carbide, as an active phase in Fe based catalysts, however, the relative rates among primary RWGS reactions, secondary CO hydrogenation to olefins and to paraffins were insensitive to the addition of Zn. Decoration of Na into Fe catalysts altered significantly the rate dependencies on both reactants and reaction temperature for olefins formation, which might be the results of the modification of the reducibility and surface identities of Fe catalysts by Na atoms, thus changed the rate ratios of paraffins and olefins. As results of decoration of Na and addition of Zn, the modified Fe based catalyst exhibits optimal performance for CO 2 hydrogenation to olefins, which shows a CO 2 conversion of 43 % with a selectivity of 54.1 % to high olefins, and a high olefins-to-paraffins ratio of 7.3.
研究领域:
催化化学
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材料科学
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DOI
高影响因子
JOURNAL OF APPLIED POLYMER SCIENCE
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2023
·Vol. 140
·期 48
·e54734
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IF 3
Haixiang Sun,Qi Jing,Yuhao Chen,Juan Liu,Haixing Ye,Ming Wang,Peng Li
Based on the solution-diffusion model of pervaporation (PV) technique, the development of thin-film composite membranes (TFC) with a highly hydrophilic surface and hydrophobic internal structure is more conducive to the rapid adsorption and desorption of water molecules to overcome the trade-off effect between flux and separation selectivity. Herein, the polyamide PV membrane was fabricated via interfacial polymerization (IP) with trimesoyl chloride (TMC) and polyethylenimine (PEI) as organic and aqueous phase monomer, respectively, on the hydrolyzed polyacrylonitrile (HPAN) substrate. Subsequently, the hydrophilic modification layer was prepared via sodium alginate (SA) crosslinking with Ca 2+ to form the egg-box network. The results indicated the optimized TFC membrane exhibited high separation factor of 525.1 with desirable permeation flux of 2083.9 g m −2 h −1 for the pervaporation dehydration 85 wt% ethanol/water solution at 70°C. The modification method of hydrophilic surface opens up new avenues for the preparation of PV membrane with high separation performance and low-cost.
研究领域:
材料科学
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化学工程
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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IF 19.503
Weifeng Tu,Chao Sun,Zhengzhou Zhang,Wenqi Liu,Haripal Singh Malhi,Wei Ma,Minghui Zhu,Yi-Fan Han
This work unravels the chemical and structural properties of Fe 5 C 2 -ZnO catalysts decorated with sodium (Na) during CO 2 hydrogenation to linear α-olefins, determined by rate assessments and series of in-situ characterizations. Reaction network remains as a combination of reverse water-gas-shift (RWGS) and CO hydrogenation, but their relative contributions vary. The RWGS reaction is chemically equilibrated, thus CO 2 conversion is determined solely by the thermodynamic constraint. However, Na addition alleviates the formation rates of paraffins from the subsequent CO hydrogenation and reactions of olefins with hydrogen. Na additive does not alter the structures of Fe 5 C 2 -ZnO, but improves largely the stability of Fe 5 C 2 by preventing the phase oxidation during the reaction. Na modifies the surface properties of catalyst, thus facilitates reaction of CO* and H* and the C C bond formation. The dual role of Na leads more effective olefins turnovers and provides new insights to the design of novel catalysts for CO 2 utilization.
研究领域:
催化化学
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材料科学
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Jiaqi Feng,Yanlin Wang,Guilin Li,Qizhou Xue,Min Wang,Xiaofu Sun,Shaojuan Zeng,Xiangping Zhang
Copper-based catalysts hold promise for electrochemical reduction of CO 2 to multi-carbon (C 2+ ) products, but achieving high selectivity and ampere-level current density remains challenging. A key hurdle lies in stabilizing Cu + species under reducing conditions, which are crucial for C-C coupling reaction. Herein, we modified Cu 2 O with sodium citrate through the coordination interaction between Cu atoms and carboxyl group. In situ spectroscopy analysis and theoretical studies revealed that the modification induced electron transfer from Cu 2 O to the citrate anion, stabilizing Cu + species under reduction conditions. Additionally, the presence of sodium citrate facilitated the hydrogenation of *CO to *CHO, with *CHO being more prone to C-C coupling reactions. Thereby, the as-prepared catalyst showed an C 2+ products Faradaic efficiency (FE) of 88.1 % at − 0.9 V vs reversible hydrogen electrode (RHE) with a C 2+ products partial current density ( j C2+ ) of 825.94 mA cm −2 and maintained over 80 % FE at − 1.1 V vs RHE with j C2+ of 1239.92 mA cm −2 . This work suggests that surface modification of Cu 2 O via carboxyl group is an effective strategy for altering the surface electronic structure of Cu 2 O and regulating the C-C coupling pathway, encouraging the exploration of more carboxyl-containing molecules for modifying copper-based catalysts to further enhance electrocatalytic performance.
研究领域:
电化学
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催化材料
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能源转换
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产品关联
DOI
高影响因子
Journal of Coatings Technology and Research
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2023
·Vol. 20
·期 5
·1513-1527
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IF 2.3
Yao Hongrui,Bi Wenya,Yin Xu,Mu Shenglong,Sha Shiqiang,Wang Na
In this work, h-BN@STPP was successfully obtained by facile co-modification of sodium tripolyphosphate (STPP) and silane coupling agent (KH-550) on h-BN nanosheets, with waterborne epoxy coatings incorporated for metallic substrate corrosion protection. Results showed that the impedance modulus at the lowest frequency ( Z f = 0.1 Hz ) of h-BN@STPP composite coating increased three orders of magnitude in comparison with neat waterborne epoxy coating, exhibiting outstanding corrosion resistance. The reinforced anticorrosion performances of h-BN@STPP composite coatings could be attributed to the “labyrinth effect” of h-BN and passivation effect of STPP on the metal substrates. Graphical abstract
研究领域:
材料科学
·
腐蚀与防护
✓ 已验证
DOI
高影响因子
FOOD HYDROCOLLOIDS
·
2024
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IF 11
Wenzhi Lei,Maodong Qi,Jiangling Song,Hongcai Li,Xingnan Wang,Yue Ma,Zhenpeng Gao
Starch nanoparticles (SNPs) have been recognized as potentially efficient adsorbents for polyphenols. However, their actual adsorption in complex systems such as fruit pomace extract is significantly lower than theoretical predictions and their adsorption capacity is inferior to traditional materials such as macroporous adsorbent resins, which limits their industrial application. Aiming to enhance the adsorption of apple pomace polyphenols, this study used sodium alginate (SA) modifies SNPs to create a cornstarch-based composite system (SA-SNPs). The optimal modified addition of sodium alginate was 0.3 g (g starch) −1 , under this condition, the nanoparticles obtained exhibited the smallest particle size (154.60 nm) and the best adsorption performance (33.97 mg g −1 in 90 min). The SA-SNPs reached the adsorption equilibrium at 180 min, which significantly enhanced the equilibrium adsorption amount of the polyphenols (from 2.68 to 37.02 mg g −1 ). The adsorption process was found to follow the pseudo-second- order kinetic model and the Langmuir isotherm model, which included membrane diffusion, intra-particle diffusion, and equilibrium phases. The adsorption amount initially increased and then continued to decrease with the increase in temperature, and the whole process was exothermic and spontaneous (ΔH° = −52.394 kJ mol −1 , ΔG° < 0 kJ mol −1 ). Additionally, SA-SNPs loaded with polyphenols demonstrated better protection of polyphenol DPPH radical-scavenging activity during storage, enhanced stability, and optimal colon-targeted sustained-release properties in complex physiological environments. This work presents a new approach to improving the adsorption capacity of SNPs and developing high-performance natural edible separation materials.
研究领域:
食品科学
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生物化学
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产品关联
DOI
高影响因子
RSC Advances
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2016
·Vol. 6
·期 17
·14329-14334
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IF 3.289
Juanjuan Li,Yang Liu,Ruitao Cha,Bei Ran,Kaiwen Mou,Huashan Wang,Qian Xie,Jiashu Sun,Xingyu Jiang
This paper reports a new synthesis method to control the size of iron oxide nanoparticles (IONs) by adding sodium citrate during fabrication to obtain sodium citrate-modified iron oxide nanoparticles (SCIONs). The method was simpler and more effective than the synthetic process of ferumoxytol, a commercial nano-sized iron agent. Compared with other iron agents which were prepared using branched polymers to form a carbohydrate shell, our SCIONs were tightly bound within a nonionic carbohydrate matrix. The physicochemical properties of SCIONs were characterized, and the results showed that these nanoparticles could be stably stored in water for six months without sedimentation. The cytotoxicity evaluation of SCIONs indicated that they were biocompatible to cells. The effect of iron supply by SCIONs was assessed by measuring the retention of iron ions in the serum, and the results demonstrated that the synthesized SCIONs are very promising for intravenous iron supply.
研究领域:
材料科学
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医学
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纳米技术
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产品关联
DOI
高影响因子
AICHE JOURNAL
·
2022
·Vol. 69
·期 5
·e17999
·
IF 4.167
Dong Lin,Yang Xu,Xiuhui Zheng,Wei Sheng,Zhenyi Liu,Yinglong Yan,Yu Cao,Yibin Liu,Xiang Feng,De Chen,Chaohe Yang
Regulating the microenvironment of active sites is crucial to boost the performance of direct propene epoxidation with H 2 and O 2 . Herein, the enhanced surface transfer of H 2 O 2 intermediates was first achieved by sodium-decorated Au-Ti bifunctional active sites. Combined with multi-techniques (e.g., operando UV–vis–NIR system, DFT studies and quantitative model calculations), it is found that the sodium-decorated silanols (Si-ONa species) on the TS-1 support enhance the formation of Ti-OOH intermediates by restraining H 2 O 2 decomposition. In addition, sodium-decorated silanols improves the desorption of propylene oxide, suppressing its ring-opening and formation for the carbonaceous deposits. Moreover, the sodium-decorated Au nanoparticles with smaller diameter and higher electron density further strengthen O 2 adsorption and boost the H 2 O 2 formation. This work not only provides fundamental understandings on the microenvironment of Au-Ti bifunctional catalysts but also sheds new light on enhancing the performance by boosting the surface molecular transfer.
研究领域:
催化化学
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材料科学
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理论计算化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Polymer Materials
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2024
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IF 4.4
Jie Wang,Jie Li,Wenfeng Luo,Qi Liu,Chen Wang,Bing Ren,Yang Cao,Jing Han,Yingchun Li
Developing conductive hydrogels with excellent low-temperature strain-sensing properties is still a challenge. In this study, sodium alginate (SA) is used as a modifier for liquid metal (LM) to construct a double network conductive hydrogel using physicochemical cross-linked quaternary ammonium salts of chitosan and core–shell LM@SA composite. The effect of sodium alginate modification on the low-temperature strain-sensing properties of liquid metal hydrogel was studied. The results show that it leads to good stretchability (stress: 1.13 MPa, strain: 382%) and strain sensing sensitivity (GF: 3.66) of composite hydrogel prepared by adding 0.3 wt % of SA. Interestingly, adding 0.3 wt % of SA is beneficial for the low-temperature (minimum temperature: −40 °C) strain-sensing enhancement of the hydrogels, which is attributed to the supercooling effect of LM by promoting the dispersion into droplets with small particle size and the reduction of the free water content by forming the hydrogen bonds between molecules. The composite hydrogel can be used as a flexible strain sensor with the ability to monitor human activities over a wide operating temperature range and as a flexible keyboard. Overall, the study presented here provides a approach for antifreezing hydrogels that can be used for wearable strain sensors.
研究领域:
材料科学
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生物医学工程
✓ 已验证
产品关联
DOI
高影响因子
Materials Today Chemistry
·
2023
·
IF 7.3
Hu Shen,Song Zhang,Mengqi Jin,Rong Liu,Dong Yang,Xin Zhou,Shengmin Wang,Zhitao Shen,Ying Liu,Fumin Li,Huilin Li,Ruirui Cao,Chong Chen
Cadmium selenide (CdSe) quantum dots (QDs) as functional interface layer have been used to improve the performances of perovskite solar cells (PSCs). However, the optimization of PSCs by CdSe QDs has some challenges of inferior performances for charge transportation, and interface defects, which are not conducive to the development of power conversion efficiency (PCE). Here, sodium thiosulfate capped CdSe QDs (S 2 O 3 2- -CdSe QDs) are prepared as interface modifiers to improve the performances of PSCs. The S 2 O 3 2- -CdSe QDs can effectively passivate defects and reduce interfacial nonradiative recombination, Moreover, the S 2 O 3 2- -CdSe QDs regulate the energy level of perovskite film. In addition, the S 2 O 3 2- -CdSe QDs form an interface layer to increase moisture resistance and improve the stability of PSCs. As a result, the devices with S 2 O 3 2- -CdSe QDs show an improved power conversion efficiency (PCE) of 22.57 %. Meanwhile, the stabilities of the unencapsulated device with S 2 O 3 2- -CdSe QDs under 25 °C with a humidity of 30 %–40 %, and 85 °C in N 2 heat both perform better than the control devices.
研究领域:
材料科学
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能源技术
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纳米科技
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）