JOURNAL OF MEMBRANE SCIENCE
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2017
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IF 6.035
Xingyu Wu,Wei Liu,Hong Wu,Xue Zong,Leixin Yang,Yingzhen Wu,Yanxiong Ren,Chengyou Shi,Shaofei Wang,Zhongyi Jiang
In this study, novel kinds of MMMs were fabricated by incorporating ZIF-67 nanoparticles into polymers of intrinsic microporosity (PIM-1). ZIF-67 (Co substituted ZIF-8) displays stiffer Co-N bond as compared with the Zn-N bond in ZIF-8, which might led to the slightly smaller effective pore aperture of ZIF-67. Good compatibility between ZIF-67 nanoparticles and PIM-1 matrix rendered ideal interfacial morphology. The intrinsic separation performance of ZIF-67 was estimated from our experimental separation results based on the Maxwell model. The calculation demonstrated its superior CO 2 /CH 4 selectivity of 45, which is twice compared with that of ZIF-8, supporting the high molecular sieving efficiency of PIM-1/ZIF-67 MMMs. Particularly, the CO 2 and H 2 permeability increased by 15.1% and 59.6% for PIM-1 membrane with 20 wt% ZIF-67 loading, meanwhile CO 2 /CH 4 and H 2 /CH 4 selectivity increased by 34.4% and 86.96%, respectively. The strategy of incorporating highly selective ZIFs into polymers of intrinsic microporosity may have promising potential in fabricating high performance membranes for efficient gas separation.
研究领域:
材料科学
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化学工程
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DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
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2025
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IF 14.3
Wenjiao Chang,Honghuo Wang,Tingting Wu,Shuting Zhang,Yifan Li,Junying Wang,Yongqiang Yang,Lei Wang
Photocatalytic CO 2 reduction reaction is regarded as a potential strategy to convert greenhouse gases into valuable chemicals. However, achieving photocatalysts with high efficiency and target product selectivity under visible light still faces great challenges. Herein, sub-2 nm RuO 2 @TiO 2 (RTO) nanorods with lattice matching interface are rationally designed and prepared via a hydrothermal reaction step-by-step. Due to the strong interaction of the lattice-matched interface with the Ru-O-Ti bond, new energy levels have emerged at the interface, leading to effective visible light absorbance. Moreover, the photo-generated electrons could be transferred to the RuO 2 efficiently via the lattice-matched interface. As a result, the RTO photocatalyst exhibits superior CO 2 -to-CH 4 conversion performance of 15.6 µmol g −1 with a selectivity of 87.9% under visible light irradiation. Density functional theory (DFT) calculation reveals that the energy barrier of CO* to CO is significantly higher than that of *CHO, resulting in the preferential production of CH 4 . This work provides an effective strategy for designing photocatalyst with promoted visible light absorption and improved product selectivity.
研究领域:
材料科学
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环境科学
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催化化学
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产品关联
DOI
高影响因子
CHEMICAL PHYSICS LETTERS
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2024
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IF 2.8
Ye Liu,Lei Zhang,Yubo Kuang,Xiaoqian Xiang,Haohan Tao,Guangran Di,Xiaojing Yin,Meicheng Li,Xiao-Jun Lv
The photocatalytic CO 2 reduction has the problems of low selectivity of single product. Here, the preparation of Cu modified tubular C 3 N 4 (CTN) was studied. The increase of the active site inhibits the recombination of electrons (e-) and holes (h + ) and improves the selectivity of CO 2 reduction products. Finally, the CO and CH 4 yields of 1.5 % CTN photocatalyst are 11.55 μmol·g −1 and 4.72 μmol·g −1 , respectively, which are 5 times higher than that of tubular C 3 N 4 photocatalyst. The selectivity of 2 % CTN to CH 4 is up to 68 %, indicating that the prepared CTN photocatalyst has high CO 2 reduction activity and CH 4 selectivity.
研究领域:
材料科学
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环境科学
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化学工程
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Ziyi Li,Jia Xiong,Yufei Huang,Yangqiang Huang,Geoffrey I.N. Waterhouse,Ziyun Wang,Yu Mao,Zhiwu Liang,Xiao Luo
Photocatalytic CO 2 reduction reaction (CO 2 RR) is usually constrained by sluggish kinetics and low product selectivity. Herein, a Cu-doping multi-tier hierarchical S-scheme heterostructure Cu-ZnIn 2 S 4 /ZIF-67 was fabricated, achieving highly efficient photocatalytic CO 2 RR under visible light without additional thermal input. At low pressure (absolute pressure 40 kPa), the optimized catalyst 2Cu-ZISF demonstrated a CH 4 yield of 22.27 μmol g −1 h −1 with a selectivity of 94.7 %. In situ XPS and EPR confirmed that the photogenerated charge transfer obeys an S-scheme mechanism, with Cu sites serving as electron-rich centers, facilitating spatial charge separation. In situ DRIFT detected reaction intermediates of photocatalytic CO 2 RR mechanism, and Gibbs free energy calculations via Density Functional Theory revealed that Cu incorporation significantly stabilizes surface CO* species, thus reducing CO(g) production and facilitating hydrogenation, thereby acting as targeted active sites for CH 4 production. This work overcomes the limitations of slow reaction kinetics and offers an in-depth understanding of how to design effective S-scheme heterojunction photocatalysts and their charge transfer mechanisms.
研究领域:
材料科学
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环境科学
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化学
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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
Zhi-Wen Wang,Qiang Wan,Ying-Zhang Shi,Huan Wang,Yue-Yue Kang,Shu-Ying Zhu,Sen Lin,Ling Wu
Ultrathin TiO 2 nanosheet (NST) with abundant Ti 3+ sites is developed as a photocatalyst which exhibits a high yield (147.2 μmol g −1 h −1 ) and selectivity (96.8%) for CO 2 to CH 4 . The results of in situ FTIR, in situ EPR and density functional theory (DFT) calculation suggest that CO 2 would be selectively activated on NST surface via forming the bridging Ti···CO 2 − ···Ti coordination species which not only lowers the activation energy barrier, but also determines the selectivity of CH 4 . Additionally, NST with the better separation and transfer ability for photogenerated electrons-holes can fleetly supply the electrons to CO 2 molecules for high efficiently producing CH 4 via the Ti-C coordination bond. Finally, a possible mechanism of the synergistic effect about coordination-activation and photocatalysis is discussed at a molecule level. This work would offer a perspective for designing an effective photocatalyst and tailoring the selectivity of products by coordination activation.
研究领域:
材料科学
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环境科学
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化学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Qiaoshan Chen,Yueling Chen,Mingfei Yu,Bin Xu,Houyi Wu,Liuyi Li,Jinhong Bi
A metal–insulator-semiconductor (MIS) ternary photo-system was intricately crafted through precise amalgamation polyvinylpyrrolidone (PVP)-capped metal Cu with typical covalent triazine framework CTF-1 via electrostatic self-assembly. The 2 % Cu-PVP-CTF exhibited an impressive CH 4 yield of 80.7 μmol·g −1 ·h −1 with selectivity of 96.8 % under visible light, representing a 2.3-fold and 112-fold improvement over Schottky-type Cu-CTF and pristine CTF-1, respectively. In-situ XPS and VASP-diff calculations unfolded that the ultrathin PVP insulating layer significantly expedited interfacial charges tunneling, corroborated by smaller lifetime τ 2 determined via femtosecond transient absorption spectroscopy. The intermediates of paramount importance in CO 2 reduction like *COOH and *HCHO were meticulously monitored by in-situ Fourier infrared spectroscopy. DFT calculations elucidated that Cu-PVP-CTF was notably more adept at facillitating the rate-determining step (*COOH → *CO) to produce CH 4 than Cu-CTF. This work tamps the groundwork for conceptional roadmap in designing novel MIS photo-system for CO 2 conversion.
研究领域:
材料科学
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催化化学
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能源转换
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产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
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2022
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IF 8.047
Wenhao Li,De-Kun Ma,Xia Hu,Faliang Gou,Xiaogang Yang,Walker MacSwain,ChenZe Qi,Weiwei Zheng
Rationally designing and controlling the interactions between reaction intermediates and the surface of photocatalysts is critical to obtain high product selectivity in photocatalysis. Herein, using CdS-based photocatalytic CO 2 reduction reaction (CO 2 RR) as a model system, we demonstrate that CH 4 selectivity can be significantly enhanced through the introduction of La 3+ ions with high oxophilicity on the surface of the photocatalysts. The high surface oxophilicity of the photocatalysts can increase CO* desorption energy and promote further hydrogenation to CH 4 . In contrast, when Au 3+ ions with low oxophilicity were doped in CdS, reduced CH 4 selectivity was observed in the CO 2 RR. Significantly, enhanced CH 4 selectivity can be achieved by doping oxophilic La 3+ ions into a broad range of alternative photocatalysts including ZnO, SnS 2 , BiOBr, BiVO 4 , TaON, and CsPbBr 3 , which demonstrates the general strategy to enhance CH 4 selectivity of photocatalytic CO 2 RR through increased surface oxophilicity of the photocatalysts by rare earth La 3+ ion doping.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
Small
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2024
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IF 13
Shuhan Fan,Qu Yang,Guilin Yin,Xiaosi Qi,Yuyu Feng,Junfei Ding,Qiong Peng,Yunpeng Qu,Qinglong Wang,Yan Shen,Mingkui Wang,Xiu Gong
Developing efficient and stable halide perovskite-based photocatalysts for highly selectivity reduction CO 2 to valuable fuels remains a significant challenge due to their intrinsic instability. Herein, a novel heterostructure featuring 2D Cs 3 Sb 2 I 9 nanosheets on a 3D flower-like mesoporous NiTiO 3 framework using a top-down stepwise membrane fabrication technique is constructed. The unique bilayer heterostructure formed on the 3D mesoporous framework endowed NiTiO 3 /Cs 3 Sb 2 I 9 with sufficient and close interface contact, minimizing charge transport distance, and effectively promoting the charge transfer at the interface, thus improving the reaction efficiency of the catalyst surface. As revealed by characterization and calculation, the coupling of Cs 3 Sb 2 I 9 with NiTiO 3 facilitates the hydrogenation process during catalytic, directing reaction intermediates toward highly selective CH 4 production. Furthermore, the van der Waals forces inherent in the 3D/2D heterostructure with face-to-face contact provide superior stability, ensuring the efficient realization of photocatalytic CO 2 reduction to CH 4 . Consequently, the optimized 3D/2D NiTiO 3 /Cs 3 Sb 2 I 9 heterostructure demonstrates an impressive CH 4 yield of 43.4 µmol g −1 h −1 with a selectivity of up to 88.6%, surpassing most reported perovskite-based photocatalysts to date. This investigation contributes to overcoming the challenges of commercializing perovskite-based photocatalysts and paves the way for the development of sustainable and efficient CO 2 conversion technologies.
研究领域:
材料科学
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环境科学
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化学工程
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产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Honglin Li,Shoufu Cao,Hongman Sun,Yonglian Lu,Ying Zhang,Xiaoqing Lu,Jingbin Zeng,Zifeng Yan
Copper (Cu) has been proved as an efficient catalyst in carbon dioxide electrochemical reduction reaction (CO 2 RR) towards hydrocarbons, but still suffers from low selectivity and poor stability. Herein, Cu-based/CxNy catalysts were fabricated by facile pyrolysis of CuNCN in sealed quartz tubes. It is found that CuNCN pyrolyzed at 300 °C (CuNCN-300) exhibits a high C 2 H 4 Faradaic efficiency of 48.5% at 500 mA cm - 2 . However, increasing the pyrolysis temperature above 400 °C gives rise to CH 4 being the predominant product and CuNCN-500 achieves CH 4 Faradaic efficiencies of 66.3% at 300 mA cm - 2 . Combining experimental and DFT calculation results, Cu 3 N plays a crucial role in the formation of C 2 H 4 , while tri-s-triazine units in CuNCN-500 reduce the barrier of *CO hydrogenation to *CHO and retard C-C coupling on Cu surface. These findings mark the significance of precise tailoring of the synergistic effect between g-C 3 N 4 and different Cu species for achieving the desired selectivity during CO 2 RR.
研究领域:
材料科学
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电化学
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理论计算
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产品关联
DOI
高影响因子
Frontiers in Chemistry
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2024
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IF 3.8
An Sufeng,Wang Peng,Wang Kuanling,Wang Xuehai,Li Baozhong,Guo Xinwen
The M/SSZ-39 catalysts (M = In, Co, Cu, Fe) with different metal species and metal loadings were synthesized using the wet impregnation method on a small-pore SSZ-39 molecular sieve. X-ray diffraction (XRD), transmission electron microscopy (TEM), nitrogen adsorption-dehydrogenation and hydrogen temperature program reduction (H2-TPR) were employed to characterize the effects of various metal components and metal loadings on the performance of CH4 selective catalytic reduction of NO reaction (CH4-SCR). The characterization results showed that the In/SSZ-39 catalyst exhibited significantly higher catalytic activity compared to the Cu-, Co-, and Fe/SSZ-39 catalysts, suggesting that indium (In) is a more suitable active ingredient for the CH4-SCR reaction. The xIn/SSZ-39 (x = 1, 2, 3, x represents the In loadings of 1.0 wt%, 2.0 wt% and 3.0 wt%) catalysts, with different In loadings, all present excellent CH4-SCR performance. By varying the In loadings, the type of In species present in the catalyst can be regulated, thus enhancing DeNOx activity and CH4 selectivity in the CH4-SCR reaction. At a low temperature of 400 °C and a low CH4/NO feed ratio (CH4/NO = 1), the 3In/SSZ-39 catalyst, featuring highly active InOx clusters, achieves the best low-temperature CH4-SCR performance, with a high NO conversion rate of up to 90% and a CH4 selectivity of up to 74.2%.
研究领域:
环境科学
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催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2019
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IF 3.372
Zihan Qu,Hong Wu,Yue Zhou,Leixin Yang,Xingyu Wu,Yingzhen Wu,Yanxiong Ren,Ning Zhang,Yutao Liu,Zhongyi Jiang
Membranes with fast CO 2 transport pathways have attracted intense attention due to their outstanding CO 2 permeability, showing potential for industrial application. Regulating the spatial distribution of CO 2 -philic groups in polymer-based membranes is expected to be a promising strategy to achieve the fast CO 2 transport pathways. In membrane matrix, the interconnected network of concentrated domains of CO 2 facilitated transport groups provides membranes with specific CO 2 transport pathways and finally leads to their high separation performance. In this study, a novel kind of polyelectrolyte membrane, quaternary ammonium polysulfone with interconnected ionic clusters, is prepared to enhance the CO 2 permeability. The hydrophilic quaternary ammonium groups tend to aggregate spontaneously to create ionic clusters. Furthermore, under humidified conditions, these ionic clusters are connected by water to form an ionic cluster network in the membrane matrix. The ionic cluster network plays the crucial role in accelerating the selective transport for CO 2 molecules over CH 4 by the reversible interaction between CO 2 and ion pairs. By tuning the quaternization degree of polysulfone, a series of polyelectrolyte membranes with different size of ionic clusters were developed. Membranes with hydrated ionic clusters (5–9 nm) show dramatic enhancement in CO 2 separation performance, especially in CO 2 permeability. The as-prepared quaternary ammonium polysulfone membrane with 8.98 nm ionic clusters exhibited the high CO 2 permeability of 1109.44 Barrer and a high CO 2 /CH 4 selectivity of 29.70, which exceeds 2008 Robeson upper bound limit. The optimized separation performance of QA-PSf membranes is attractive for potential application such as CO 2 capture from flue gas and natural gas.
研究领域:
材料科学
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化学工程
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环境科学
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产品关联
DOI
高影响因子
CATALYSIS COMMUNICATIONS
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2023
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IF 3.7
Jiuhu Zhao,Huiying Li,Yungang Wang,Rongshu Zhu,Senlin Sun,Jingwen Zhang,Chaolin Li,Mei Hong
Mesoporous In/Hβ-X series catalysts were prepared by desilication method with tetrapropylammonium hydroxide (TPAOH) and indium incorporation for selective catalytic reduction of NO with methane (CH 4 -SCR). The post desilication treatment conditions for preparing In/Hβ-X were optimized. Etching time is the most important desilication parameter influencing the resulting CH 4 -SCR performance of the catalyst. The In/Hβ-3 sample which was etched for 3 h presents the highest NO x conversion, 22% higher than In/H-Beta counterparts using commercial microporous beta. Obvious analysis reveals that besides generating mesopores, controlled desilication can modulate the proportion of InO + active sites and surface oxygen species, allowing more active sites to be exposed.
研究领域:
催化
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环境科学
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化学工程
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）