Journal of CO2 Utilization
·
2022
·
IF 8.321
Nicui Yuan,Yuxin Mei,Yuwei Liu,Yating Xie,Baining Lin,Yonghua Zhou
The development of efficient and highly selective photocatalysts is a key point for the photocatalytic conversion of CO 2 . In this paper, a composite catalyst UiO-66-NH 2 /Ce(HCOO) 3 (simplified to UNH/Ce(HCOO) 3 ) was fabricated by one pot method with CeCO 3 OH as the precursor. Scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS) characterizations results confirmed that UNH was dispersed on the surface of Ce(HCOO) 3 and strongly interacted with it via Ce-N bond. The yield of CH 4 on the optimal UNH/Ce(HCOO) 3 catalyst reached 3 times of that on pristine UNH, up to 128.81 μmol g −1 , with the CH 4 selectivity of 71.9 %, and the R electron reached 286.46 μmol g −1 h −1 . The UV–vis diffuse reflection spectra and photoelectrochemical tests results confirmed that the improved photocatalytic CO 2 reduction performance and high CH 4 selectivity could be attributed to the formation of the type-Ⅱheterojunction of UNH/Ce(HCOO) 3 with abundant Ce 3+ , which expanded the visible light absorption range, accelerated the separation and transfer rates of photogenerated charges, and thus efficiently promoted the multi-electron reduction reaction of CO 2 to CH 4 . In addition, the reaction temperature affected profoundly the cycle performance of the catalyst. The results presented here illustrated the possibility for improving the stability of UNH/Ce(HCOO) 3 -1.80 by decreasing reaction temperature.
研究领域:
材料科学
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环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
INORGANIC CHEMISTRY
·
2021
·
IF 5.165
Ziqi Zhou,Ruibiao Fu,Qirui Shui,Hongxin Tang,Wenxiu Bao,Zuju Ma,Xintao Wu
Nonlinear optical (NLO) materials are playing an increasingly vital role in laser science and technology. Herein, we report a new lead formate, KCs2Pb2(HCOO)2Cl5, successfully synthesized by using mild mix-solvothermal methods. By the anionic substitution of a [CH3COO] group with a [HCOO] group, the dipole moment of the distorted [PbCl4O2] polyhedron is increased. In contrast, polarization from the anionic group and the volume of the unit cell are reduced. Hence, KCs2Pb2(HCOO)2Cl5 possesses a strong second-harmonic-generation (SHG) response of 4.2 times that of KH2PO4 (KDP), a transparent window covering 0.43–1.87 μm, a large band gap of 3.52 eV, and moderate birefringence (0.11@1064 nm). Systematic theoretical calculations illustrate the origin of the linear and nonlinear optical properties of KCs2Pb2(HCOO)2Cl5. This research provides a viable strategy for the design and synthesis of new NLO crystals.
研究领域:
材料科学
·
光学
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2024
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IF 6.3
Huiyuan Cheng,Jingwei Hu,Zihan Liu,Guangping Lei,Guojun Xi,Yayun Zhang,Hantao Liu,Xuhuan Guo,Huiyun Ren
Developing novel adsorbents for CO 2 capture and separation offers an efficient approach to relieving global environmental problems. To promote CO 2 capture from flue gas, novel Cr 3 O@MIL-101(Cr) composites was synthesized through packing [Cr 3 O(HCOO) 6 (H 2 O) 3 ]NO 3 into MIL-101(Cr) cages. The resultant composite Cr 3 O@MIL-101(Cr) presents higher CO 2 uptakes at lower pressure ranges, benefiting from the increased content of unsaturated Cr(III) ions and micropores relative to MIL-101(Cr). Meanwhile, IAST selectivity for CO 2 /N 2 mixture reached 50.2 under standard temperature and pressure, outperforming most of the reported materials. Further GCMC simulations reveal that the synergistic effect of [Cr 3 O(HCOO) 6 (H 2 O) 3 ] + , NO 3 − and MIL-101 (Cr) could effectively facilitate the interactions with CO 2 molecules and hinder N 2 molecules from approaching the optimal adsorption sites. Thus the [Cr 3 O(HCOO) 6 (H 2 O) 3 ]NO 3 encapsulated MIL-101(Cr) can be recommended as a promising adsorbent for superior CO 2 /N 2 separation.
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
产品关联
DOI
高影响因子
Frontiers of Chemical Science and Engineering
·
2024
·Vol. 18
·期 11
·1-10
·
IF 4.3
Liang Haoting,Zhao Qiao,Liu Shengkun,Wei Chongyang,Wang Yidan,Wang Yue,Huang Shouying,Ma Xinbin
The Fe-Mn bimetallic catalyst is a potential candidate for the conversion of CO 2 into value-added chemicals. The interaction between the two metals plays a significant role in determining the catalytic performance, however which remains controversial. In this study, we aim to investigate the impact of tuning the proximity of Fe-Mn bimetallic catalysts with similar nanoparticle size. And its effect on the physicochemical properties of the catalysts and corresponding performance were investigated. It was found that closer Fe-Mn proximity resulted in enhanced CO 2 hydrogenation activity and inhibited CH 4 formation. The physiochemical properties of prepared catalysts were characterized using X-ray diffraction, H 2 temperature programmed reduction, and X-ray photoelectron spectroscopy, revealing that a closer Fe-Mn distance promoted electron transfer from Mn to Fe, thereby facilitating Fe carburization. The adsorption behavior of CO 2 and the identification of reaction intermediates were analyzed using CO 2 -temperature programed desorption and in situ Fourier transform infrared spectroscopy, confirming the intimate Fe-Mn sites contributed to CO 2 adsorption and the formation of HCOO* species, ultimately leading to increased CO 2 conversion and hydrocarbon production. The discovery of a synergistic effect at the intimate Fe-Mn sites in this study provides valuable insights into the relationship between active sites and promoters.
研究领域:
催化化学
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材料科学
✓ 已验证
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
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2025
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IF 2.5
Xiude Peng,Xiaohua Cao,Huaiyu Xu,Ruibin Xiong,Dedong He,Dingkai Chen,Yongming Luo
CO2-ODHP has been demonstrated to be an effective technology for the production of propylene. CO2 acts as a soft oxidizer that reduces over-oxidation of hydrocarbons and improves propylene selectivity. However, CO2-ODHP still faces the challenge of rapid catalyst deactivation due to coke accumulation at elevated operating temperatures. Herein, we prepared a La-modified Ga/ZSM-5 catalyst, in which La modified the acidic–basic properties of Ga/ZSM-5 and improved the resistance to coke accumulation of the catalyst. The synthesized Ga2La1/ZSM-5 catalyst achieved propane conversion up to 80% at 580 °C. In situ DRIFTS analysis revealed that the addition of La could significantly accelerate the formation of HCOO* intermediates, which further improved the efficiency of the CO2-ODHP reaction.
研究领域:
化学工程
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Bio Materials
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2020
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IF 0
Xinke Kong,Panpan Gai,Feng Li
Biohybrid photoelectrochemical systems could combine the light-harvesting ability of semiconductor photocatalysts and the CO2-processing capability of biocatalysts to realize CO2 reduction. How to develop the energy-utilized model can be of importance for the mechanism exploration of photosynthesis. Here, a biohybrid photoelectrochemical system based on HCOO––CO2 circulation was developed to realize the conversion both of solar-to-electric energy and chemical-to-electric energy. The device consists of a TiO2 nanoparticle photoanode and a laser-scribed graphene/formate dehydrogenase biocathode, which was utilized for the formic acid oxidation and the biocatalysis reduction of CO2 to HCOO–, respectively. The as-proposed biohybrid photoelectrochemical system exhibits good performance with an open-circuit potential of 0.93 V and a maximum power output density of 76 μW cm–2. This ingenious strategy not only exploits a robust carbon circulation system for the conversion of solar energy but also provides a way of constructing complex artificial photosynthesis systems.
研究领域:
生物技术
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能源科学
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环境科学
✓ 已验证
DOI
DALTON TRANSACTIONS
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2023
·Vol. 52
·期 46
·17273-17278
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IF 4
Li Zhang,Hong-Lin Zhu,Zhong-Yi Li,Yue-Qing Zheng
The exploitation of highly active and stable catalysts for reduction of CO2 and water oxidation is one of the approaches to facilitate scalable and sustainable CO2 reduction potentially at the industrial scale. Herein, a feasible strategy to rationally build an overall CO2 + H2O electrocatalytic reaction device is the preparation and matchup of a high-performance CO2 reduction catalyst and low-cost and highly active oxygen anode catalyst. A heterostructured nanosheet, γ-NiOOH/NiCO3/Ni(HCOO)2, exhibited superior catalytic activity in the oxygen evolution reaction, and was integrated with CoPc/Fe–N–C to build an overall CO2 + H2O cell with a current density of 10 mA cm−2 at a very low cell voltage of 1.97 V, and the faradaic deficiency of CO2 to CO was maintained at greater than 90% at 1.9 V.
研究领域:
能源化学
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催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
·
IF 9.1
Hongfei Ma,Yanfang Huang,Yufei Xie,Wenjuan Wang,Guihong Han
Developing materials that combine ultrahigh adsorption capacity with facile solid–liquid separation remains a central challenge in interfacial science for fluoride pollution control. Current research on metal-organic frameworks (MOFs) as adsorption carriers mainly emphasizes structural design, while byproducts generated during MOF synthesis are commonly regarded as useless impurities and consequently neglected. Herein, we report a previously overlooked crystalline byproduct, La(HCOO) 3 , which was initially formed via N , N -dimethylformamide (DMF) hydrolysis during the solvothermal synthesis of La-BDC and can be subsequently controllably synthesized by the deliberate introduction of formic acid. Owing to its uniform and well-defined particle size, La(HCOO) 3 can be readily separated from La-BDC by simple physical sieving, enabling its direct recovery. Inspired by this feature, we propose a “waste-to-resource” strategy by directly employing La(HCOO) 3 as a functional material for fluoride adsorption flotation for the first time. Under optimized conditions, La(HCOO) 3 exhibits a fluoride adsorption efficiency of 96.29% and a flotation separation efficiency of 94.22%, yielding a low effluent turbidity of 4.37 NTU and excellent selectivity. The adsorption process follows a monolayer chemisorption model with a maximum theoretical adsorption capacity of 206.61 mg/g, outperforming many deliberately designed adsorption carriers. Combined characterization and density functional theory (DFT) calculation reveal that fluoride adsorption is governed by the synergistic effects of ligand exchange and electrostatic attraction, while sodium dodecyl sulfate (SDS) enables efficient flotation recovery through chemical adsorption and electrostatic interactions with La(III) sites. This study reveals a novel approach for the interfacial valorization of MOF byproducts and a sustainable route for fluoride remediation.
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DOI
高影响因子
CHEMICAL ENGINEERING & TECHNOLOGY
·
2017
·Vol. 41
·期 2
·353-366
·
IF 2.051
Shumin Wang,Qingping Guo,Shujun Liang,Peng Li,Xin Li,Jujie Luo
For the evaluation of CH 4 /N 2 separation, mixed-matrix membranes (MMMs) were fabricated by adding [Ni 3 (HCOO) 6 ] as a filler into the poly(styrene- b -butadiene- b -styrene) (SBS) polymer. The structures and morphologies of [Ni 3 (HCOO) 6 ] and [Ni 3 (HCOO) 6 ]/SBS MMMs were characterized by different techniques, proving the crystalline structure of [Ni 3 (HCOO) 6 ] in SBS polymer matrices. The structural integrity of the MMMs and good compatibility between [Ni 3 (HCOO) 6 ] and SBS polymer were examined by scanning electron microscopy. Gas permeation measurements revealed that membranes containing various [Ni 3 (HCOO) 6 ] loadings exhibited different separation performances. The operational temperature exerted a significantly positive effect on the separation of CH 4 and N 2 .
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DOI
高影响因子
Advanced Science
·
2024
·
IF 14.3
Jinxian Feng,Chunfa Liu,Lulu Qiao,Keyu An,Sen Lin,Weng Fai Ip,Hui Pan
Electrolyte plays crucial roles in electrochemical CO 2 reduction reaction (e-CO 2 RR), yet how it affects the e-CO 2 RR performance still being unclarified. In this work, it is reported that Sn-Zn hybrid oxide enables excellent CO 2 -to-HCOO − conversion in KHCO 3 with a HCOO − Faraday efficiency ≈89%, a yield rate ≈0.58 mmol cm −2 h −1 and a stability up to ≈60 h at −0.93 V, which are higher than those in NaHCO 3 and K 2 SO 4 . Systematical characterizations unveil that the surface reconstruction on Sn-Zn greatly depends on the electrolyte using: the Sn-SnO 2 /ZnO, the ZnO encapsulated Sn-SnO 2 /ZnO and the Sn-SnO 2 /Zn-ZnO are reconstructed on the surface by KHCO 3 , NaHCO 3 and K 2 SO 4 , respectively. The improved CO 2 -to-HCOO − performance in KHCO 3 is highly attributed to the reconstructed Sn-SnO 2 /ZnO, which can enhance the charge transportation, promote the CO 2 adsorption and optimize the adsorption configuration, accumulate the protons by enhancing water adsorption/cleavage and limit the hydrogen evolution. The findings may provide insightful understanding on the relationship between electrolyte and surface reconstruction in e-CO 2 RR and guide the design of novel electrocatalyst for effective CO 2 reduction.
研究领域:
电化学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Green Energy & Environment
·
2024
·
IF 10.7
Junming Zeng,Yongbin Yao,Fang Wang,Jiajian Gao,Lili Zhang,Guangwen Xu,Ziyi Zhong,Fabing Su
Nickle-based catalysts are commonly used for CO 2 methanation. However, there is still potential to improve their catalytic performance under mild conditions. In this study, we synthesized a series of Ru-Ni-Al catalysts from Ru-doped NiAl-hydrotalcite using a hydrothermal method. The Ru-Ni-Al catalyst demonstrated much higher activity for CO 2 methanation than the Ni-Al catalyst that did not have Ru doping. Both experimental results and theoretical calculations indicate that the enhanced performance of the Ru-Ni-Al catalyst is related to electronic interactions between nickel (Ni) and ruthenium (Ru). The Ru sites transfer electrons to the Ni sites, increasing the local electron density of Ni, which enhances the adsorption and activation of H 2 . Furthermore, the Ru-Ni metal interface sites improve the adsorption and activation of CO 2 . In situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS) analysis indicates that adjusting the electronic structure of Ni sites can accelerate the production of intermediates HCOO*, while Ru-Ni intermetallic interface sites can directly dissociate CO 2 into CO*. In addition, CO 2 methanation on the Ru-Ni-Al catalyst follows HCOO*- and CO*-mediated pathways. This study underscores the potential for enhancing CO 2 methanation performance by modulating the electronic structure of Ni sites.
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
产品关联
DOI
高影响因子
Functional Materials Letters
·
2018
·
IF 1.084
Jujie Luo,Xing Yang,Shumin Wang,Yuhong Bi,Amit Nautiyal,Xinyu Zhang
The metal organic framework (MOF) [Ni 3 (HCOO) 6 ] was synthesized via the simple and fast microwave method, and the effect of irradiation power on crystallinity of synthesized Ni-based MOF was studied. The samples were characterized by using Fourier Transform Infrared Spectroscopy (FTIR), X-ray diffraction (XRD), and scanning electron microscopy (SEM). The synthesized Ni-based MOF was electrochemically characterized by using galvanostatic charge–discharge (GCD), cyclic voltammetry (CV), and electrochemical impedance spectroscopy (EIS) techniques. The synthesized MOF showed the highest specific capacitance of 1196.2 F/g at 1 A/g with excellent cyclability (86.04% capacitance retention after 2,000 cycles), thereby demonstrating its potential application in supercapacitors.
研究领域:
材料科学
·
电化学
✓ 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）