MOLECULES
·
2024
·Vol. 29
·期 8
·1899
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IF 4.2
Jun Wang,Shuang Fu,Peng Hou,Jun Liu,Chao Li,Hongguang Zhang,Guowei Wang
Utilizing solar energy for photocatalytic CO2reduction is an attractive research field because of its convenience, safety, and practicality. The selection of an appropriate photocatalyst is the key to achieve efficient CO2reduction. Herein, we report the synthesis of TiO2/CuPc heterojunctions by compositing CuPc with TiO2microspheres via a hydroxyl-induced self-assembly process. The experimental investigations demonstrated that the optimal TiO2/0.5CuPc photocatalyst exhibited a significantly enhanced CO2photoreduction rate up to 32.4 μmol·g−1·h−1under 300 W xenon lamp irradiation, which was 3.7 times that of the TiO2microspheres alone. The results of photoelectrochemical experiments indicated that the construction of the heterojunctions by introducing CuPc effectively promoted the separation and transport of photogenerated carriers, thus enhancing the catalytic effect of the photocatalyst.
研究领域:
材料科学
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMISTRY OF MATERIALS
·
2025
·
IF 7
Beibei Sun,Cheng Zeng,Suyun Deng,Yuewen Gu,Lei Gan,Huajun Yang
The separation of C2H2/CO2 under highly humid conditions by using metal–organic frameworks (MOFs) is extremely challenging because water vapor would reduce the C2H2 adsorption capacity or even degrade the structure of MOFs. In this work, a zirconium zeolitic metal–organic framework (NNM-5) with a small aperture and large cavities exhibits commendable C2H2/CO2 selectivity (16.6 at 298 K and 1 bar) and a high uptake ratio (3.13 at 298 K and 1 bar). More importantly, NNM-5 could maintain at least five breakthrough cycles under highly humid conditions (around 100% RH) without performance degradation compared to that under dry conditions. Our studies indicate that the kinetic mechanism is the key to excellent separation performance under highly humid conditions based on the fact that the material is hydrophilic with a high water uptake, but the diffusion rate of H2O is 2 orders slower than that of C2H2 and CO2 in NNM-5.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
Nano Research
·
2024
·Vol. 17
·期 9
·7945-7956
·
IF 9.5
Li Ting,Zhang Zhen-Yu,Luo De-Cun,Xu Bo-Yu,Zhang Rong-Jiang,Yao Ji-Long,Li Dan,Xie Tao
Solar-driven photo-thermal catalytic CO 2 methanation reaction is a promising technology to alleviate the problems posed by greenhouse gases emissions. However, designing advanced photo-thermal catalysts remains a research challenge for CO 2 methanation reaction. In this work, a series of ABO 3 (A = lanthanide, B = transition metal) perovskite catalysts with Ce-substituted LaNiO 3 (La 1− x Ce x NiO 3 , x = 0, 0.2, 0.5, 0.8, 1) were synthesized for CO 2 methanation. The La 0.2 Ce 0.8 NiO 3 exhibited the highest CH 4 formation rate of 258.9 mmol·g −1 ·h cat −1 , CO 2 conversion of 55.4% and 97.2% CH 4 selectivity at 300 °C with the light intensity of 2.9 W·cm −2 . Then the catalysts were thoroughly analyzed by physicochemical structure and optical properties characterizations. The partial substitution of the A-site provided more active sites for the adsorption and activation of CO 2 /H 2 . The sources of the active sites were considered to be the oxygen vacancies (O v ) created by lattice distortions due to different species of ions (La 3+ , Ce 4+ , Ce 3+ ) and exsolved Ni 0 by H 2 reduction. The catalysts have excellent light absorption absorbance and low electron–hole (e − /h + ) recombination rate, which greatly contribute to the excellent performance in photo-thermal synergistic catalysis (PTC) CO 2 methanation. The results of in situ irradiated electron paramagnetic resonance spectrometer (ISI-EPR) and ISI-X-ray photoelectron spectroscopy (XPS) indicated that the aggregation of unpaired electrons near the defects and Ni metal (from La and Ce ions to O v and Ni 0 ) accelerated adsorption and activation of CO 2 /H 2 . At last, the catalyst properties and structure were correlated with the proposed reaction mechanism from the in situ diffuse reflection infrared Fourier transform spectrum (DRIFTS) measurements. The in situ precipitation of the B-site enhanced the dispersion of Ni, while its enriched photoelectrons upon illumination further promote hydrogen dissociation. More H* spillover accelerated the rate-determining step (RDS) of HCOO* hydrogenation. This work provides the theoretical basis for the development of catalysts and industrial application.
研究领域:
材料科学
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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
Surfaces and Interfaces
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2025
·
IF 6.3
Jintao Zhou,Yan Liu,Chuncheng Yang,Guoyong Wang
Doping and interface engineering are both pivotal strategies for enhancing the selectivity of CO 2 reduction catalysts. However, as these strategies have often been explored independently, the question of which is more effective or whether their effects can be synergistically combined remains open. Given that doping and interfaces serve as crystallographic defects, they can be engineered to coexist within the same crystal structure. In this study, we strategically introduced both defects into a copper catalyst by modulating the indium content during crystal growth. Our investigation into the electrochemical performance of these catalysts for CO conversion reveals that while doping consistently enhances conversion selectivity, the presence of Cu/In interfaces disrupts this trend. The most promising catalyst, with 3% indium doping, demonstrated an impressive CO selectivity of 95.38±1.5% and a partial current density of -2.25 mA cm - ² at -0.8 V vs. Reversible Hydrogen Electrode (RHE). This research provides critical insights into the complex interplay between doping and interface engineering, offering a new pathway for the rational design of highly selective CO 2 reduction catalysts.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of CO2 Utilization
·
2018
·
IF 5.503
Jianyang Wang,Anfeng Zhang,Xiao Jiang,Chunshan Song,Xinwen Guo
Although many researchers have reported CO 2 hydrogenation to various C1 chemicals, it is still challenging to directly and selectively convert CO 2 to C 2 -C 4 hydrocarbons in terms of overcoming the extreme inertness of CO 2 and a high C C coupling barrier. In the present work, we report an efficient integration of methanol-synthesis and the methanol-to-hydrocarbons with the bifunctional catalyst component of In 2 O 3 -ZrO 2 and SAPO-5. These tandem reactions exhibit an excellent relative selectivity of C 2 -C 4 (83%) with a suppressed CH 4 relative selectivity less than 3% at T = 300 °C. A detailed analysis indicates that the partially reduced indium oxide surface (In 2 O 3 -ZrO 2 ) can better activate CO 2 and promote the synthesis of methanol than In 2 O 3 alone, and C C coupling is subsequently manipulated within the confined acidic pores of SAPO-5 according to XRD, H 2 -TPR, CO 2 -TPD, SEM and TEM. Furthermore, the proximity of two components and the content of Si also play an important role in such outstanding selectivity to C 2 -C 4 . Our study paves a new path for the direct synthesis of lower hydrocarbons.
研究领域:
化学工程
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催化化学
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能源化学
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS TODAY
·
2019
·
IF 4.888
Lei Zhang,Hao Wang,Chengguang Yang,Xiaopeng Li,Jian Sun,Hui Wang,Peng Gao,Yuhan Sun
The present work reports on the promoting effects of rare earth elements (La, Ce and Y) to FeK/Al 2 O 3 catalysts on liquid hydrocarbons from CO 2 hydrogenation. The addition of La, Ce and Y can both improve the selectivity of C 5+ hydrocarbons and reduce the selectivity of CH 4 . The C 5+ selectivity can enhance to about 60 % with CH 4 selectivity of around 11 % at CO 2 conversions above 20 %. N 2 adsorption–desorption, in situ XRD, H 2 –TPR, CO 2 /H 2 –TPD, HRTEM and XPS are used to characterize the FeK/Al 2 O 3 and FeK/M-Al 2 O 3 (M = La, Ce, Y) catalysts. The results show that the introduction of rare earth elements into the FeK/Al 2 O 3 catalyst obviously reduces the adsorption of H 2 , which suppresses the CH 4 formation. On the other hand, rare earth elements also promote the adsorbed CO 2 species, which leads to the enhanced liquid hydrocarbons selectivity. Finally, the tailored CO 2 /H 2 ratio of CO 2 and H 2 adsorption on the catalyst surface can influence the catalyst activity and the product selectivity evidently.
研究领域:
催化化学
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材料科学
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环境科学
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2018
·
IF 3.909
Jiawen Chen,Shuning Chen,Wei Cheng,Jinhuo Lin,Shisheng Hou,Haiqing Liu,Qinhui Chen
Effective control of bleeding is critical to saving lives whether on the battle field or in civilian life. Microporous starch (MS) is a promising hemostat for its extensive sources, huge surface area and good biocompatibility. However, the hemostatic performance of MS is limited because of its complex preparation process and lack of effective component to activate coagulation factors . Herein, porous starch microspheres modified by calcium (Ca-PSM) with dense shell and honeycomb micro-porous core were prepared by electrostatic spray and supercritical CO 2 for the first time. The topological morphology of Ca-PSM changed with the increase of Tween-80 content within 0.5%. Ca-PSM possessed excellent water absorbability due to high specific surface area, and what's more, it showed good hemostatic performance because of the synergistic effects of physical adsorption and chemical activation mechanisms. The results of thrombelastograph (TEG) showed that the initial clotting time (R) and coagulation time (R + K) of Ca-PSM-1 were shortened by 47.1%, 53.3% than that of control group. The maximum blood clot strength (MA) of Ca-PSM-1 was also significantly raised. Furthermore, it was noteworthy that Ca-PSM could activate clotting cascade and induce erythrocyte adsorption. In summary, Ca-PSM as a hemostat will be a promising and alternative candidate for clinical application.
研究领域:
生物材料学
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医学工程
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药剂学
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Xiaoqian Li,Dechao Wang,Hailong Ning,Yangyang Xin,Zhongjie He,Fangfang Su,Yudeng Wang,Jing Zhang,Hongni Wang,Liwei Qian,Yaping Zheng,Dongdong Yao,Mingtao Li
Porous liquids (PLs), as a novel liquid sorbent with permanent porosity, still present challenges such as high viscosity and melting temperatures. Herein, an efficient electrostatic repulsion strategy is proposed to engineer zeolitic imidazolate frameworks (ZIFs) type III PLs employing ZIF-8- g -BPEI nanoparticle stability dispersed into BPEI. The viscosity and melting temperatures of ZIF-8- g -BPEI PLs could be tailored via control particle size, grafting polymer, and concentration of porous nanoparticles . The existence of BPEI on the surface of ZIF-8- g -BPEI facilitates the stable dispersion of ZIFs nanoparticles in BPEI via the electrostatic repulsion as well as enhances CO 2 adsorption capacity of PLs. Moreover, the CO 2 adsorption amount of ZIF-8- g -BPEI-30 PLs is 6.5 times high than that of neat BPEI, suggesting the permanent free volume of ZIFs is retained in their corresponding PLs. Benefiting from the branched structure of BPEI grafted onto the outer surface of ZIFs , ZIF-8- g -BPEI-10 PLs remain liquified down to -71.1 °C, together with viscosity as 1.7 Pa·s −1 at 25 °C. Therefore, the electrostatic repulsion strategy opens an effective avenue to prepare novel liquid materials and shows numerous potential applications in gas adsorption and separation.
研究领域:
材料科学
·
环境科学
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 42
·23817-23827
·
IF 12.732
Manman Feng,Xuemei Wu,Huiyuan Cheng,Zihao Fan,Xiangcun Li,Fujun Cui,Shuai Fan,Yan Dai,Guangping Lei,Gaohong He
The diatomic catalysts (DACs) provide a new strategy for efficient catalysis of CO2 reduction reaction (CO2RR) owing to their maximum atomic utility and more flexible active sites. However, it is still challenging to precisely design heteronuclear diatomic active centers and understand the coordination mechanism of binary sites at the atomic level. Herein, a nitrogen-doped carbon matrix with precisely controlled Fe–Cu diatom sites is synthesized through a metal–organic framework. The as-obtained Fe/Cu–N–C catalyst exhibits an excellent CO faradaic efficiency (>95% over a wide potential range of −0.4 to −1.1 V vs. RHE, 99.2% at −0.8 V vs. RHE), a high turnover frequency (5047 h−1 at −1.1 V vs. RHE), and a low overpotential (50 mV), thus outperforming most reported atomically dispersed catalysts. Further density functional theory calculations indicate that the synergy between Fe–Cu diatoms causes rapid charge transfer and effectively adjusts the position of the d-band center, which reduces the energy barriers for *COOH formation and *CO desorption. This work provides a new approach for advancing universal synthesis strategies to construct heteronuclear diatomic catalysts and explore synergistic effects.
研究领域:
材料科学
·
催化化学
·
能源转换
✓ 已验证
DOI
高影响因子
CHEMOSPHERE
·
2020
·
IF 5.778
Dong Xia,Ange Maurice,Antoine Leybros,Jong-Min Lee,Agnes Grandjean,Jean-Christophe P. Gabriel
Removal of brominated flame retardants (BFRs) from polymers before disposal or recycling will alleviate negative environmental effects and ensure safe usage of recycled products. Extraction of BFRs in supercritical CO 2 is appealing but also presents challenges to industries due to limited solubility and lack of kinetic studies. For a more comprehensive evaluation of supercritical extraction potentialities, we (i) developed an on-line pressure apparatus that is compatible with both the FTIR and UV–vis spectrometers to enable kinetic and thermodynamic studies; (ii) studied kinetic extraction involving three conventional and two novel BFRs as well as three typical polymeric matrix. Solubilities were determined using the gravimetric method or X-ray fluorescence. FTIR exhibited a superior applicability compared to UV–vis in the following BFR extraction’s time-dependency binary and ternary systems . We observed that faster stirring speed, higher temperature, and finer particle size can accelerate the overall extraction kinetics. In binary systems, it took less than 2 h to achieve equilibrium for each BFR at 60 °C, 25 MPa and 1000 rpm. In the presence of polymeric matrix, slower extraction kinetics were observed due to the occurrence of competitive dissolution and molecular diffusion within the matrix. Mathematical models derived from irreversible desorption and Fick’s diffusion laws fitted well with the observed extraction kinetics of BFRs, thus enabling us to identify the rate-determining step. The high solubilization rate coefficients that we measured for BFRs revealed that the dynamic extraction process in up-scaling design could compensate for the low solubility with flowing supercritical CO 2 .
研究领域:
环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING
·
2025
·
IF 4.6
Yulin Tan,Ziye Shen,Ying Yang,Huimin Zhang,Yufang Xie,Chenglin Zhang,Yuan Liu,Mingming Chen,Dawei Cao
Heterojunction engineering significantly enhances photocatalytic CO 2 reduction performance. However, a large lattice mismatch in heterostructures hinders photocatalytic reaction by forming extensive grain boundaries, inefficient interfaces, and sluggish interfacial charge transfer. Metal halide perovskites, featuring soft lattices induced by weak ionic metal-halide bonds, offer effective solutions to alleviate such mismatches. Herein, we fabricate BaTiO 3 /CsPbBr 3 photocatalysts with a precisely engineered type-II heterojunction. Notably, the BaTiO 3 /CsPbBr 3 heterostructure achieves a CO formation rate of 17.3 μmol∙g −1 h −1 — 5.2-fold and 2.3-fold higher than pristine BaTiO 3 (3.3 μmol∙g −1 h −1 ) and CsPbBr 3 (7.6 μmol∙g −1 h −1 ), respectively. This improvement stems from the synergistic effect of enhanced light absorption and charge separation. This work provides fundamental insights for developing high-performance heterojunction photocatalysts.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Yadong Du,Xiangtong Meng,Jun Qi,Benxiang Gong,Yangjun Ma,Jiachun Li,Hongqi Zou,Jieshan Qiu
Electrochemical CO 2 reduction (ECR) to value-added products provides a pathway to reduce CO 2 emission and to enable a closed carbon cycle. Compared to powdered catalysts, self-supporting electrocatalysts have more prominent advantages such as high charge transfer capacity and the ability to serve directly as working electrodes without the need for binders. Herein, a self-supporting catalyst featuring SnO 2 nanoparticles incorporated into porous carbon nanofiber (SnO 2 -PCNF) was crafted via electrospinning followed by annealing in CO 2 . SnO 2 -PCNF can directly function as working electrode for ECR to produce HCOOH, achieving a high Faradaic efficiency of 92.3%. Also, the SnO 2 -PCNF can stably catalyze ECR process for more than 50 h. Theoretical calculations and in-situ Raman spectroscopy elucidate the underlying ECR mechanism over SnO 2 -PCNF, wherein the catalyst significantly reduces the energy barrier of the rate-determining step. This effectively suppresses the competitive hydrogen generation. This work provides some insights into design of binder-free and high-performance ECR electrocatalysts.
研究领域:
材料科学
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环境科学
·
能源化学
✓ 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）