Journal of Environmental Sciences
·
2023
·
IF 6.9
Junying Yi,Yuli Chen,Dongze Lai,Bihong Lv,Xiaomin Wu,Guohua Jing
Bi 2 O 3 catalyst with Bi-O bond crystal structure has more active sites, which shows better CO 2 catalytic performance than pure Bi catalysts in many catalytic reactions. How to strengthen the Bi-O bond in Bi 2 O 3 to obtain higher selectivity and catalytic activity is a problem worthy of consideration. Here, we develop a N 2 pre-reduced spherical Bi 2 O 3 /ATO catalyst that has a high formate Faradaic efficiency of 92.7%, which is superior to the existing tin oxide catalyst. Detailed electrocatalytic analysis shows that N 2 pre-reduction and spherical structure are helpful for Sn to stabilize the oxidation state of Bi, thus retaining part of the Bi-O structure. The existence of the Bi-O structure can reduce the energy barrier of the CO 2 production *OCHO reaction and promote the reaction rate of the CO 2 -*OCHO-HCOOH path, thus promoting the formation of formate.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yue Chen,Meigui He,Jianmin Zhang,Yiting Su,Zhe Xue,Chengze He,Yufan Ji,Kecheng Guan,Jing Zhao,Hideto Matsuyama,Wanqin Jin
Cross-linked poly(ethylene oxide) (PEO) is a highly promising membrane material for CO 2 capture, as it allows fast and selective CO 2 transport. However, the facile fabrication of an ultrathin cross-linked PEO selective layer for thin-film composite (TFC) membrane to achieve high CO 2 separation performance remains challenging. To address this issue, we reported the design of a soluble high-permeability cross-linked PEO polymer and the fabrication of it into an ultrathin CO 2 -selective layer through a simple coating technique. The as-synthesized cross-linked PEO polymer contains abundant poly(dimethylsiloxane) (PDMS) segments, leading to highly improved free volume and affinity towards CO 2 , which result in high CO 2 diffusivity, solubility, and consequently high CO 2 permeability (528 Barrer). TFC membranes with an ultrathin selective layer (∼128 nm) were successfully fabricated using the PEO polymer, leading to superior CO 2 capture performance (CO 2 permeance = 2650 GPU, CO 2 /N 2 = 20) for CO 2 /N 2 mixture separation in a long-term stability test, exceeding the target performance for carbon capture. Given their high separation performance, excellent stability, and scalable fabrication route, our PEO-based membranes hold great promise for post-combustion CO 2 capture.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Shitao Han,Wei Xia,Shuaiqiang Jia,Jiapeng Jiao,Ting Yao,Xue Dong,Min Wang,Jianxin Zhai,Jiahao Yang,Yijun Xie,Xueqing Xing,Haihong Wu,Mingyuan He,Buxing Han
Electrochemical CO 2 reduction reaction (CO 2 RR) using renewable energy to produce valuable multicarbon (C 2+ ) products is a promising approach for carbon emission reduction. In this work, we propose a new strategy to enhance the formation of hydrogen-containing intermediates using the excellent abilities of proton transportation and electronic structure modification of phosphorus (P). To realize this, an in situ electrodeposition method was proposed to prepare P-doped Cu catalysts. It was found that the electrodeposition potential significantly impacts the structure and catalytic performance of P-Cu catalysts. Specifically, the catalyst obtained at − 0.5 V vs. Ag/AgCl exhibited exceptional performance for CO 2 RR towards C 2+ products, achieving a Faradaic efficiency (FE) of ∼ 80.2 % and a partial current density of 40.4 mA cm −2 in an H-type cell. Furthermore, the catalyst demonstrated stability for at least 12 h. Experimental and density functional theory (DFT) studies revealed that the free energy of the hydrogenated process could be significantly reduced by the excellent proton transport ability of P, and the interaction of Cu with the unpaired electrons of carbon could be improved, leading to excellent adsorption ability of Cu for the intermediates and high FE of C 2+ products.
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ACS Catalysis
·
2023
·
IF 12.9
Xuanyu Yue,Duojia Zheng,Ming Gao,Ke Wang,Zizhong Zhang,Wenxin Dai,Xianzhi Fu
The direct decomposition of CO2 to produce CO and O2 requires extremely high temperatures in catalysis. Here, we proposed the photoassisted oxygen vacancy active sites for CO2 dissociation to lower the reaction temperature. The designed low-crystalline Nb2O5 nanoribbons (LC-Nb2O5 NRs) showed a good CO production rate under mild conditions (≤250 °C) with Xe lamp irradiation. Under light irradiation, the rate of CO yields of LC-Nb2O5 NRs increased to 68 μmol g–1 h–1 at 250 °C, with no activity at all under light conditions. The high activity arose from unsaturated coordination with low crystallinity and CO2 reactants as an electron donor for forming an electron cycle with the Nb2O5 NRs, which played a key role in the generation of oxygen vacancies for the subsequent photoexcited electron transfer process at mild temperatures. The feasibility of this approach is further verified over Nb2O5/C nanofibers that make full use of photothermal and photoelectric effects to achieve long-term stable CO2 decomposition.
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JOURNAL OF MEMBRANE SCIENCE
·
2023
·
IF 9.5
Xiaohui Liu,Boyu Li,Jiaxiang Liu,Xuanting He,Huachen Liu,Shun Mao,Wenquan Tao,Zhuo Li
Membrane separation technology has been widely used in the separation and capture of CO 2 to reduce carbon emissions. The performances of facilitated hybrid membranes (FHMs) can be improved by properly adding metal-organic framework (MOF)-based nanoparticles (NPs) and modifying polymers to the polymer matrix . Grafting and blending methods are widely used to introduce modifying polymers to improve the compatibility between NPs and the polymer matrix, and the performance of FHMs for CO 2 separation. However, the separation performance of FHMs decreases significantly when the long chains of the polymer infiltrate into the pores of the MOF at the interface between the modifying polymer and MOF. To in-depth understand the nano-scale polymer-NPs interfacial interaction mechanism of the grafting and blending methods, we herein employed molecular dynamic (MD) simulation method combined with experiments to investigate the interface between NPs of Cu-MOF (Cu-BDC) and four commonly used modifying polymers (PEG, polyethylene glycol; PEI , polyethylenimine; PVA , polyvinyl alcohol; PPy, polypyrrole) with PVDF (polyvinylidene difluoride) as the polymer matrix. The results showed that the blending method for modification can effectively avoid the polymer blockage in Cu-BDC pores by using four modifying polymers, while the grafting method caused polymer infiltration for PEG and PEI. The relationship between the polymer diameter and the pore limiting diameter (PLD) of the Cu-BDC was evaluated to analyze the polymer infiltration effect. FHMs of Cu-BDC/PEG@PVDF were synthesized based on the MD simulation results, which showed excellent CO 2 separation performance due to the good compatibility between the Cu-BDC and the modified matrix polymer. This work offers an insight in nano-scale into the interface design between the MOF and the polymer for FHMs separating CO 2 .
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Petroleum Science
·
2023
·
IF 5.6
Xi-Dao Wu,Peng Xiao,Bei Liu,Guang-Jin Chen,Jian-Hua Pang
CO 2 emulsions used for EOR have received a lot of interest because of its good performance on CO 2 mobility reduction. However, most of them have been focusing on the high quality CO 2 emulsion (high CO 2 fraction), while CO 2 emulsion with high water cut has been rarely researched. In this paper, we carried out a comprehensive experimental study of using high water cut CO 2 /H 2 O emulsion for enhancing oil recovery. Firstly, a nonionic surfactant, alkyl glycosides (APG), was selected to stabilize CO 2 /H 2 O emulsion, and the corresponding morphology and stability were evaluated with a transparent PVT cell. Subsequently, plugging capacity and apparent viscosity of CO 2 /H 2 O emulsion were measured systematically by a sand pack displacement apparatus connected with a 1.95-m long capillary tube. Furthermore, a high water cut (40 vol%) CO 2 /H 2 O emulsion was selected for flooding experiments in a long sand pack and a core sample, and the oil recovery, the rate of oil recovery, and the pressure gradients were analyzed. The results indicated that APG had a good performance on emulsifying and stabilizing CO 2 emulsion. An inversion from H 2 O/CO 2 emulsion to CO 2 /H 2 O emulsion with the increase in water cut was confirmed. CO 2 /H 2 O emulsions with lower water cuts presented higher apparent viscosity, while the optimal plugging capacity of CO 2 /H 2 O emulsion occurred at a certain water cut. Eventually, the displacement using CO 2 /H 2 O emulsion provided 18.98% and 13.36% additional oil recovery than that using pure CO 2 in long sand pack and core tests, respectively. This work may provide guidelines for EOR using CO 2 emulsions with high water cut.
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Journal of Environmental Chemical Engineering
·
2023
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IF 7.7
Jinghao Hua,Sheng Feng,Changchang Ma,Haitao Huang,Kai Wei,Xiaojun Dai,Kaidi Wu,Haihong Wang,Zhaowei Bian
In this study, a novel 2D/2D Z-scheme Bi 5 O 7 Br/NiFe-LDH photocatalyst was prepared by combining NiFe-LDH with Bi 5 O 7 Br through self-assembly. Under simulated solar irradiation, compared with pure NiFe-LDH and Bi 5 O 7 Br, the 2D/2D Z-scheme Bi 5 O 7 Br/NiFe-LDH photocatalyst revealed a significant improvement in the efficiency of photocatalytic reduction of CO 2 . Z-scheme heterojunction promotes the separation of photo generated charge carriers and 2D/2D structure is conducive to exposing more active site and enhancing the migration rate of interface carriers. The photocatalytic activity experiment revealed that the CH 4 production efficiency of the Bi 5 O 7 Br/NiFe-LDH (37.77 μmol/g/h) after 8 h of light exposure was 2 times and 10 times that of Bi 5 O 7 Br (22.41 μmol/g/h) and NiFe-LDH (3.84 μmol/g/h), respectively. The successful formation of Z-scheme heterojunction was determined through band analysis and related characterization. The advantage of Z-scheme heterojunction is that it has high electron mobility and low resistivity. This work launches a feasible design strategy of special structure photocatalysts to enhance the photocatalytic activity for the CO 2 reduction.
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PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
·
2023
·Vol. 120
·期 44
·e2307320120
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IF 11.1
Yangyang Yu,Ye He,Ping Yan,Shengyao Wang,Fan Dong
The selective photocatalytic conversion of CO2 and H2O to high value-added C2H4 remains a great challenge, mainly attributed to the difficulties in C–C coupling of reaction intermediates and desorption of C2H4* intermediates from the catalyst surface. These two key issues can be simultaneously overcome by alloying Ag with Cu which gives enhanced activity to both reactions. Herein, we developed a facile stepwise photodeposition strategy to load Cu–Ag alloy sub-nanoclusters (ASNCs) on TiO2 for CO2 photoreduction to produce C2H4. The optimized catalyst exhibits a record-high C2H4 formation rate (1110.6 ± 82.5 μmol g−1 h−1) with selectivity of 49.1 ± 1.9%, which is an order-of-magnitude enhancement relative to current work for C2H4 photosynthesis. The in situ FT-IR spectra combined with DFT calculations reveal the synergistic effect of Cu and Ag in Cu–Ag ASNCs, which enable an excellent C–C coupling capability like Ag and promoted C2H4* desorption property like Cu, thus advancing the selective and efficient production of C2H4. The present work provides a deeper understanding on cluster chemistry and C–C coupling mechanism for CO2 reduction on ASNCs and develops a feasible strategy for photoreduction CO2 to C2 fuels or industrial feedstocks.
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JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
·
2023
·Vol. 99
·期 1
·183-194
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IF 3.4
Zhen Wang,Zhitao Han,Gang Liu,Zelu Zhou,Xi Wu,Song Zhou,Xinxiang Pan
BACKGROUND The large-scale practical application of CO 2 capture using carbonate solutions is mainly limited by their low CO 2 absorption rate. In view of this, it is feasible to improve CO 2 capture performance of carbonate solution by adding additives. In this paper, low-cost sodium carbonate (Na 2 CO 3 ) solution was selected as the main CO 2 absorbent, and the effects of different organic additives on CO 2 capture performance of Na 2 CO 3 solutions were systematically investigated. RESULTS The results showed that 0.04 mol/L tetrabutylammonium bromide (TBAB) could achieve a better enhancement effect on CO 2 capture performance of Na 2 CO 3 solution. After addition of TBAB, the maximum CO 2 absorption rate of Na 2 CO 3 solution was improved to 2.52 × 10 −3 mol/min, which increased by 105%. And the maximum CO 2 desorption rate could also be improved by 45%. TBAB/Na 2 CO 3 system not only realized a high CO 2 absorption capacity of 0.769 mol/mol, but also maintained 82% of the initial CO 2 absorption capacity after three cyclic tests. The regeneration heat duty of TBAB/Na 2 CO 3 solution was calculated to be 1136.6 kJ/mol, which was significantly lower than that of single Na 2 CO 3 solution and conventional MEA aqueous solution. The promotion mechanism of TBAB in Na 2 CO 3 solution was explored using Fourier transform infrared spectra (FTIR) and 13 C nuclear magnetic resonance (NMR) analysis. CONCLUSION The introduction of TBAB additive could significantly improve CO 2 capture performance of Na 2 CO 3 solution and reduce regeneration heat duty, making it a possible option in the field of post-combustion CO 2 capture. © 2023 Society of Chemical Industry (SCI).
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Chenchen Qin,Li Xu,Jian Zhang,Jun Wang,Jiaxin He,Daomeng Liu,Jia Yang,Juan-Ding Xiao,Xifan Chen,Hong-Bao Li,Zhengkun Yang,Junzhong Wang
Electroreduction of carbon dioxide into readily collectable and high-value carbon-based fuels is greatly significant to overcome the energy and environmental crises yet challenging in the development of robust and highly efficient electrocatalysts. Herein, a bismuth (Bi) heterophase electrode with enriched amorphous/crystalline interfaces was fabricated via cathodically in situ transformation of Bi-based metal-phenolic complexes (Bi-tannic acid, Bi-TA). Compared with amorphous or crystalline Bi catalyst, the amorphous/crystalline structure Bi leads to significantly enhanced performance for CO2 electroreduction. In a liquid-phase H-type cell, the Faraday efficiency (FE) of formate formation is over 90% in a wide potential range from −0.8 to −1.3 V, demonstrating a high selectivity toward formate. Moreover, in a flow cell, a large current density reaching 600 mA cm–2 can further be rendered for formate production. Theoretical calculations indicate that the amorphous/crystalline Bi heterophase interface exhibits a favorable adsorption of CO2 and lower energy barriers for the rate-determining step compared with the crystalline Bi counterparts, thus accelerating the reaction process. This work paves the way for the rational design of advanced heterointerface catalysts for CO2 reduction.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Xiaohong Ma,Jiajia Zheng,Huacheng Jin,Xi Zeng,Danyang Li,Feifei You,Jian Qi,Fangli Yuan
The utilization of solar energy to convert CO 2 into small energy molecules is a potential “carbon neutral” technology for CO 2 emission reduction. However, the industrial application is significantly constrained due to the low reduction efficiency, complexity of the synthesis methods, and limitations in scaling up the catalyst materials. In this work, we have successfully designed and synthesized a series of hollow tubular ZnO@ZnS core-sheath heterostructured materials, by combining radio-frequency thermal plasma and hydrothermal treatment technologies. The S:Zn molar ratio, reaction time, and temperature were systematically investigated, and the morphology of intermediate products was successfully captured, which provided conclusive evidence for the proposed formation mechanism. Notably, the photocatalytic CO yield of the ZS 0.5 O hollow nanotube core-sheath composite is not only 3.20 or 4.03 times higher than that of the pure ZnO or ZnS, respectively, but also possesses excellent stability. By in-depth characterization, we found that the hollow core-sheath heterostructure enhances light capture and absorption, exposes more effective active sites, and builds a type-II heterojunction between ZnO and ZnS to enhance the separation efficiency of charge carriers. The synergy of these factors significantly improves the catalytic performance, offering new insights for photocatalytic, electrocatalytic, and photoelectrocatalytic CO 2 reduction.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Haiyan Jiang,Tingting Li,Lu Bai,Jiuli Han,Xiaochun Zhang,Haifeng Dong,Shaojuan Zeng,Shuangjiang Luo,Xiangping Zhang
An efficient separation technology involving ammonia (NH3) and carbon dioxide (CO2) is of great importance for achieving low-carbon economy, environmental protection, and resource utilization. However, directly separating NH3 and CO2 for ammonia-based CO2 capture processes is still a great challenge. Herein, we propose a new strategy for selective separation of NH3 and CO2 by functional hybrid membranes that integrate polyimide (PI) and ionic liquids (ILs). The incorporated protic IL [Bim][NTf2] is confined in the interchain segment of PI, which decreases the fractional free volume and narrows the gas transport channel, benefiting the high separation selectivity of hybrid membranes. At the same time, the confined IL also provides high NH3 affinity for transport channels, promoting NH3 selective and fast transport owing to strong hydrogen bonding interaction between [Bim][NTf2] and NH3 molecules. Thus, the optimal hybrid membrane exhibits an ultrahigh NH3/CO2 ideal selectivity of up to 159 at 30 °C without sacrificing permeability, which is 60 times higher than that of the neat PI membrane and superior to the state-of-the art reported values. Moreover, the introduction of [Bim][NTf2] also reduces the permeation active energy of NH3 and reverses the hybrid membrane toward “NH3 affinity”, as understood by studying the effect of temperature. Also, NH3 molecules are much easier to transport at high temperature, showing great application potential in direct NH3/CO2 separation. Overall, this work provides a promising ultraselective membrane material for ammonia-based CO2 capture processes.
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