Environmental Science-Nano
·
2024
·
IF 5.8
Jingwei Hong,Wanli Li,Jin Shang,Hiromi Yamashita,Yun Hu
Utilizing electrocatalysis to convert CO2 into high-value industrial raw materials can not only effectively reduce CO2 emissions but also achieve a closed carbon cycle. This method holds great potential for addressing global warming and alleviating the fossil fuel crisis. Here, we report a novel electrocatalyst for CO2 reduction composed of a composite material derived from Cu-MOF74 and Cu2O, synthesized under the regulation of an appropriate amount of KOH. The research results indicate that the unique Cu0/Cu+ interface in Cu-MOF74/Cu2O-350 enhances the adsorption of reaction intermediates, providing more active sites for CO2 reduction. Additionally, the moderate carbonization during the thermal treatment process increases conductivity and enriches the electrochemical active surface area, accelerating the charge transfer rate. Consequently, this composite exhibits excellent CO2 reduction performance. At -1.3 V vs. RHE, the Faraday efficiency (FE) for C2H4 production reached up to 32.48%, which was significantly higher than that of pure Cu2O-350 (9.25%) and Cu-MOF74-350 (15.52%). Even after 6 hours of reaction, the FE for C2H4 remained above 24.52%, reflecting its good stability. Furthermore, we utilized in-situ infrared spectroscopy to study the key intermediates of the relevant reduction products, inferring the possible reaction pathways for the formation of HCOOH and C2H4. This study provides a simple synthesis method for the preparation of high-selectivity MOF-derived composite catalysts for the electrocatalytic reduction of CO2 to value-added chemicals.
研究领域:
电化学
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材料科学
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环境科学
·
催化
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Miao Sun,Xiao Xu,Shihao Min,Jiaxin He,Kun Li,Longtian Kang
Copper-based metal-organic framework (Cu-MOF) materials with multiple active sites have attracted increasing attention to the electrocatalytic CO 2 reduction reaction (ECR), however, face the huge challenge owing to the poor stability and low C 2 selectivity. Here, the Cu 2 O/Cu-CuTCPP heterojunction (Cu 2 O/CPFs) with three Cu active sites are firstly constructed through in-situ electrodeposition method. The effect of CuSO 4 concentration and electrodeposition conditions on ECR is systematically investigated. The optimized Cu 2 O/CPFs composite achieves the ethylene Faraday efficiency (FE C2H4 ) of 61.8 % at –1.3 V vs. RHE, which is 1.9 and 3.42 times higher than those of CPFs and Cu 2 O, respectively. Meanwhile, the C 2 H 4 partial current density ( j C2H4 ) of –7.96 mA·cm −2 is 2.91 and 4.68 times higher than those of CPFs and Cu 2 O. Further experiments reveals that the formation of Cu 2+ –O–Cu + –O bond between Cu 2 O and Cu–O 4 sites in Cu 2 O/CPF heterojunction is crucial. Consequently, the hydrogen (H 2 ), formic acid (HCOOH) and methane (CH 4 ) evolution reactions are restricted, the C–C coupling reaction of *CHO and *CO intermediates is significantly enhanced, and the Cu–O 4 sites in CPFs are protected. This work provides an effective strategy to stabilize MOF structure and obtain high value-added C 2+ products.
研究领域:
材料科学
·
电化学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2024
·
IF 4.1
Hongwei Chen,Xiangqiong Jiang,Binyu Wang,Yongheng Ren,Bin Zhang,Jiabao Gui,Xili Cui,Linbing Sun,Jiuxing Jiang,Wenfu Yan,Jinping Li,Libo Li
Utilizing physical adsorption for ethylene purification from complex mixtures can significantly reduce the energy cost for production. The purification of multi-component systems through a single adsorption process presents a considerable challenge, largely stemming from the absence of customized strategies and thorough investigations into adsorption behaviours. We aim to understand adsorbents through a unique cage recognition approach and leverage these insights to develop an effective purification adsorbent, with the successful synthesis of SSZ-16 zeolite meeting requirements for multi-component purification. This zeolite, featuring a long aft supercage and a narrow gme cage construct two adsorption cages. The dense π -electron cloud of C 2 H 2 enables a stronger interaction in aft cage, while CO 2 is selectively captured within the environmentally compatible gme cage, demonstrating significantly higher C 2 H 2 and CO 2 adsorption capacity. The separation experiments reveal that SSZ-16 exhibits exceptional performance, with an unprecedented polymer-grade C 2 H 4 productivity of 2099.16 L/kg from the CO 2 /C 2 H 2 /C 2 H 4 mixture.
研究领域:
化学工程
·
材料科学
✓ 已验证
DOI
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
·
2024
·
IF 4
Di-Ming Chen,Han-Dong Qiao,Meng-Yao Sun,Shao-Ming Fang
Ethylene is an important chemical raw material which is widely used in the production of chemical fibers, plastics, rubber, coatings, as well as medicines, and its separation from the gas mixtures of C 2 H 6 /C 2 H 4 is of great importance but a challenging task due to their similar physical properties and molecular dimensions. Herein, we report the C 2 H 6 and C 2 H 4 sorption studies on a robust anionic metal-organic framework (MOF) {(NH 2 Me 2 )[Co 3 (μ 3 OH)(TPT)(TZB) 3 ](H 2 O) 6 (DMA) 6 } n (Co-MOF) formed by connection of Co 3 (OH) clusters by two N-rich organic ligands 2,4,6-tri(4-pyridyl)-1,3,5-triazine (TPT) and 4-(1H-Tetrazol-5-yl)benzoic acid (H 2 TZB). The prepared Co-MOF features a polyhedron stacking network structure composed of trigonal bipyramidal cages and octahedral cage which both contribute to a high C 2 H 6 uptake capacity of 6.48 mmol/g and a decent C 2 H 6 /C 2 H 4 selectivity of 1.54 at 298 K and 1 bar. Grand Canonical Monte Carlo (GCMC) simulation results agree well with the experimental tendency, both in the adsorption isotherms and sorption heats, which demonstrated that the suitable pore surfaces with electronegative donor sites generated multiple C H ⋅⋅⋅O/N and C H ⋅⋅⋅π interactions between the framework and C 2 H 6 , resulting in a stronger interaction between the MOF skeleton and C 2 H 6 molecule than C 2 H 4 as reflected by the dispersion-corrected density functional theory (DFT) calculation.
研究领域:
化学工程
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2024
·Vol. 48
·期 23
·10577-10583
·
IF 2.7
Kuo Zhang,Jing-Jing Pang,Xin Lian,Zi-Han Song,Yue-Chao Yuan,Hongliang Huang,Zhao-Quan Yao,Jian Xu
Separation of the mixture of ethylene (C2H4) and ethane (C2H6) to produce polymer-grade C2H4 is of prime importance in the petrochemical industry. In this context, metal–organic frameworks (MOFs) featuring tunable pore metrics and surface chemistry, especially those with inverse C2H6/C2H4 adsorption selectivity, hold great promise in energy-effective purification of C2H4 by adsorptive separation, but often encounter the well-known trade-off between adsorption selectivity and capacity. In this work, we report two new MOFs by deploying the pore-space-partition (PSP) strategy for the purpose of reducing the pore aperture size while retaining the gas-accessible pore volume. As a result, Ni-bodc-tpt (bodc = bicyclo[2.2.2]octane-1,4-dicarboxylic acid, tpt = 2,4,6-tri(4-pyridyl)-1,3,5-triazine) by combining optimal pore size, large cage pore volume, and rich C–H binding sites exhibits concurrently high C2H6 adsorption capacity (131.65 cm3 g−1) and C2H6/C2H4 selectivity (1.8) at 298 K and 1 bar, which is superior or comparable to many benchmark C2H6-selective MOFs. A dynamic breakthrough experiment demonstrates that high-purity C2H4 (>99.9%) can be harvested in one step from a binary mixture of C2H6/C2H4 (50/50, v/v), attesting to the feasibility of this new MOF as a prospective C2H4 purification agent.
研究领域:
材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2025
·
IF 4.8
Jianhao Li,Zhicheng Hu,Shuhuan Han,Dapeng Cao,Xiaofei Zeng,Jianfeng Chen
Electrocatalytic CO 2 reduction reaction (CO 2 RR) to multi-carbon product, especially for ethylene (C 2 H 4 ), provides a favorable pathway for carbon neutrality and renewable energy storage. However, the second-order C-C coupling reactions in CO 2 RR need always the high activation/driven energy in dynamics originating from the trace C 1 intermediate product. Herein, we synthesized the Ag-decorated Cu 2 O porous hollow core-shell catalyst named Ag@Cu 2 O where Ag nanoparticles uniformly distributed on inner the surface of the hollow Cu 2 O (H-Cu 2 O) via the sacrificial template method. Benefiting from the synergistic hollow structure and electron transfer from Cu and Ag to O, Ag@Cu 2 O catalyst delivers the excellent C 2 H 4 Faradaic Efficiency (FE) of 55 % ± 2 % at −1.0 V (vs. RHE), which is superior to the most reported catalysts. More importantly, in situ infrared spectroscopy and density functional theory (DFT) calculations reveal the introduction of Ag can decrease the activation energy required for *CO and C-C coupling.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2026
·
IF 8.2
Tianlong Tan,Hai Liu,Wenlong Cao,Lei Yang,Shujing Ju,Caiyu Chen,Ewald Janssens,Guowei Han,Dachun Lu,Jue Wang,Qinfang Zhang
The electrochemical CO2 reduction reaction (CO2RR) is one of the most promising pathways to achieving carbon neutrality. However, in acidic electrolytes, the CO2RR tends to suffer from competitive hydrogen evolution side reactions. Alkaline electrolytes are typically employed to suppress side reactions and promote the formation of valuable multicarbon (C2+) products (e.g., ethylene(C2H4)). In this study, we fabricated surface-loaded copper cluster catalysts with particle sizes below 5 nm by magnetron sputtering and inert gas condensation in combination with cluster beam deposition. This approach enabled precise control over the catalyst surface structure, allowing for in-depth investigation of the synergistic effects between the catalyst microstructure and its catalytic microenvironment. We demonstrate that the Faradaic efficiency (FE) for CO2-to-C2H4 conversion exceeds 50% across a broad current density range of 50 to 180 mA cm–2 in a flow cell using 1 M KOH electrolyte. Compared with a pristine Cu/PTFE catalyst, the optimized Cu cluster catalyst not only exhibits a significant enhancement in FEC2H4 but also expands the effective current density range. Furthermore, finite element simulations combined with in situ Raman spectroscopy reveal synergistic interactions among interfacial species (e.g., *CO, OH–, and K+). Therefore, this study proposes a general strategy to regulate the dynamic evolution of catalytic interfaces through an initial nanostructure design, thereby opening a promising avenue for the selective conversion of CO2 to ethylene.
✓ 已验证
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2026
·
IF 19.7
Peiyi Cao,Lizhi Tang,Zhihong Wang,Jun Wei,Jun He,Hongyun Luo,Hongjing Chen,Wenjin Cheng,Yu Yu,Weicheng Yan,Zhongkai Xie,Weidong Shi
Dual-layer system design and photothermal catalysis without external heat supply. • Exceptional catalytic performance and selectivity. • Exploring the mechanism of thermally-assisted photocatalysis. The photocatalytic conversion of CO 2 and H 2 O into C 2 H 4 is a promising approach for carbon recycling, yet current systems are limited by inefficient solar energy utilization, which confines C 2 H 4 production to micromolar levels. To address this challenge, photo-thermal catalysis was developed. The Ti 3 C 2 T x MXenes substrate, characterized by broad-spectrum solar absorption and ultralow mid-infrared emissivity, provides efficient photothermal conversion, raising the local reaction temperature and accelerating both molecular diffusion and charge carrier migration, which integration enhances the C-C coupling efficiency, leading to a remarkable 1.35 mmol·g -1 ·h -1 of C 2 H 4 production rate and 75.1% of C 2 H 4 selectivity, which surpasses the current benchmarks for photocatalytic CO 2 -to-C 2 H 4 conversion. Moreover, when deployed in a custom-designed outdoor reactor equipped with a Fresnel lens concentrator and a continuous gas flow system, the catalyst delivered up to 11.3 mL of C 2 H 4 with a total CO 2 single-pass conversion rate of 2.6% after 8 h. These results not only establish a new benchmark for photocatalytic CO 2 -to-C 2 H 4 conversion but also provide valuable insights into the cooperative mechanisms of photochemical and photothermal processes, paving the way for advanced artificial photosynthesis technologies. Download: Download high-res image (253KB) Download: Download full-size image The findings reveal cooperative mechanisms between photothermal and photocatalytic processes, establishing a generalizable design principle for advanced catalysts aimed at improving solar-to-chemical energy conversion and enabling more efficient artificial photosynthesis.
✓ 已验证
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Lu Bai,Fangxu Fan,Zeyuan Gao,Tianyou Li,Yuao Wang,Zehua Li,Rongyu Lu,Ziyu Huai,Xinyue Wu,Gaohong He,Canghai Ma
The structure of polymer precursors critically determines the performance of carbon molecular sieve (CMS) membranes, yet the role of hydroxyl-containing, thermally rearrangeable units in polyimides remains underexplored. In this work, hydroxylated 6FDA-HAB and non-hydroxylated 6FDA-DABP were employed to systematically investigate the effect of benzimidazole formation on CMS structure and ethylene/ethane separation. Thermal rearrangement (TR) affects both graphitization and microporous architecture: low TR temperatures yield amorphous, low-porosity membranes, moderate TR temperatures enhance conjugated aromatic formation and molecular sieving, while excessively high TR temperatures induce densification that reduces permeability and selectivity. The TR400 membrane pyrolyzed at 800 °C achieved a C 2 H 4 permeability of 204.6 Barrer and a C 2 H 4 /C 2 H 6 selectivity of 15.8, surpassing the latest upper bounds. These findings elucidate the pivotal role of thermally rearranged structures and provide a rational strategy for designing high-performance CMS membranes for C 2 H 4 /C 2 H 6 separation.
研究领域:
材料科学
·
膜分离技术
·
高分子化学
·
气体分离
·
纳米多孔材料
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2020
·
IF 3.573
Tengjiao He,Yonghou Xiao,Qidong Zhao,Mengxue Zhou,Gaohong He
Separation of carbon dioxide (CO2) from a CO2/ethylene (C2H4) mixture represents an important and challenging field in industrial applications. Selective adsorption has become an attractive option as an energy-saving and environmentally friendly CO2 capture technology. In this work, an ultramicroporous metal–organic framework (MOF) Qc-5-Cu was prepared by solution method and applied for the highly selective separation of CO2 from an C2H4 stream. The performance of Qc-5-Cu was evaluated by static and dynamic adsorption experiments. It was found that the single-component adsorption capacities of CO2 and C2H4 on Qc-5-Cu at 298 K and 1 bar were 2.48 and 0.74 mmol/g, respectively. The measured breakthrough curves further illustrate that Qc-5-Cu could effectively separate CO2 from the C2H4 stream for more than 10 cycles. The pore size of the obtained Qc-5-Cu was ∼3.3 Å, as characterized by nitrogen adsorption. The ultramicroporous structure of Qc-5-Cu benefits the separation of CO2, as evidenced by the selectivity values of the CO2/C2H4 binary mixture (1:99, v/v) based on the ideal adsorbed solution theory (SIAST ≈ 39.95 avg.), which are larger than some MOFs with open metal sites, owing to the weak interaction between organic ligands with high aromaticity and C2H4, as well as the porous screening effect of Qc-5-Cu on ethylene. The observed high selectivity, excellent stability, and regeneration performance demonstrate that Qc-5-Cu is a promising adsorbent for the separation of the CO2/C2H4 mixture.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
ChemSusChem
·
2023
·Vol. 16
·期 19
·e202300601
·
IF 8.4
Jilin Liu,Kai Yu,Zhiyuan Qiao,Qianlong Zhu,Hong Zhang,Jie Jiang
Graphical A tandem catalyst, Cu 2 O NCs-C-Copc, consisting of acetylene black, cobalt phthalocyanine (Copc) and Cu 2 O nanocubes was developed for efficient converting of CO 2 to C 2 H 4 . We propose the Cu 2 O NCs-C-Copc mechanism suppressing side reactions and simultaneously enriching CO. Here, we report faradaic efficiencies of C 2 H 4 formation of up to 58.42 % at −1.1 V vs. RHE in 0.1 M KHCO 3 and 70.31 % at −0.76 V vs. RHE in 1.0 M KOH. Suppressing side reactions and simultaneously enriching key intermediates during CO 2 reduction reaction (CO 2 RR) has been a challenge. Here, we propose a tandem catalyst (Cu 2 O NCs-C-Copc) consisting of acetylene black, cobalt phthalocyanine (Copc) and cuprous oxide nanocubes (Cu 2 O NCs) for efficient CO 2 -to-ethylene conversion. Density-functional theory (DFT) calculation combined with experimental verification demonstrated that Copc can provide abundant CO to nearby copper sites while acetylene black successfully reduces the formation energies of key intermediates, leading to enhanced C 2 H 4 selectivity. X-ray photoelectron spectroscopy (XPS) and potentiostatic tests indicated that the catalytic stability of Cu 2 O NCs-C-Copc was significantly enhanced compared with Cu 2 O NCs. Finally, the industrial application prospect of the catalyst was evaluated using gas diffusion electrolyzers. The of Cu 2 O NCs-C-Copc can reach to 58.4 % at −1.1 V vs. RHE in 0.1 M KHCO 3 and 70.3 % at −0.76 V vs. RHE in 1.0 M KOH. This study sheds new light on the design and development of highly efficient CO 2 RR tandem catalytic systems.
研究领域:
材料科学
·
电化学
·
催化反应
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Xianbin Xu,Difei Xiao,Yugang Gao,Wenbo Li,Miaomiao Gao,Shuang Zhao,Zeyan Wang,Zhaoke Zheng,Peng Wang,Hefeng Cheng,Yuanyuan Liu,Ying Dai,Baibiao Huang
Electrocatalytic CO2 reduction reaction (CO2RR) to high value-added products, such as ethylene (C2H4), offers a promising approach to achieve carbon neutrality. Although recent studies have reported that a tandem catalyst (for example, Cu–Ag systems) exhibits advantage in C2H4 production, its practical application is largely inhibited by the following: (1) a traditional tandem catalyst cannot effectively stabilize the *CO intermediate, resulting in sluggish C–C coupling, and (2) inadequate H2O activation ability hinders the hydrogenation of intermediates. To break through the above bottleneck, herein, palladium (Pd) was introduced into Cu2O–Ag, a typical conventional tandem catalyst, to construct a Cu2O–Pd–Ag ternary catalyst. Extensive experiment and density functional theory calculation prove that Pd can efficiently stabilize the *CO intermediate and promote the H2O activation, which contributes to the C–C coupling and intermediate hydrogenation, the key steps in the conversion of CO2 to C2H4. Beneficial to the efficient synergy of Cu2O, Pd, and Ag, the optimal Cu2O–Pd–Ag ternary catalyst achieves CO2RR toward C2H4 with a faradaic efficiency of 63.2% at −1.2 VRHE, which is higher than that achieved by Cu2O–Ag and most of other reported catalysts. This work is a fruitful exploration of a rare ternary catalyst, providing a new route for constructing an efficient CO2RR electrocatalyst.
研究领域:
材料科学
·
催化化学
·
能源转化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
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