ENERGY
·
2022
·
IF 8.857
Kun Fu,Mingzhen Zheng,Dong Fu
The results of beaker experiments (Fu et al., 2021, 2022) showed that water-lean 2-ethylhexan-1-amine (EHA) + diglyme absorbent has more advantages than the commercial water-based ethanolamine (MEA) absorbent in terms of characteristics of carbon dioxide (CO 2 ) absorption and desorption. Verifying CO 2 capture characteristics in a tower facility is essential to absorbents development. In this work, a pilot packed tower was set up and the Dg16 type polypropylene step ring was taken as packing to test the capture efficiency and mass transfer performance of EHA + diglyme water-lean absorbent for low partial pressure CO 2 , and then the effects of gas-liquid ratio, CO 2 partial pressure and packing height on the capture performance were clarified. The results showed that the absorption of CO 2 by EHA + diglyme water-lean absorbent was dominated by liquid-phase mass transfer in the packed tower. Compared with aqueous 30 wt%MEA, the water-lean EHA + diglyme achieved much higher CO 2 capture efficiency and overall volumetric mass transfer coefficient. This work demonstrated the transition from water-free absorption to water-lean absorption under the existence of water vapor in flue gas . It can provide basic data for the design of the CO 2 capture process based on water-lean absorption in packed towers.
✓ 已验证
产品关联
DOI
高影响因子
ACS Nanoscience Au
·
2026
·
IF 7.5
Guangtao Wang,Simin Li,Chao Yu,Yang Zhou,Wenlei Zhu,Bo Shen
Abstract Facet engineering of Cu-based nanocatalysts is a promising strategy for regulating the selectivity of CO2 and CO electroreduction because surface atomic arrangements strongly influence intermediate adsorption and reaction pathways. Compared with low-index facets, high-index facets contain abundant steps, kinks, and low-coordinated atoms, providing diverse active ensembles that can facilitate CO adsorption and subsequent C–C coupling. However, the catalytic roles of high-index-faceted Cu nanocatalysts remain largely unexplored. Herein, tetrahexahedral (THH) and hexoctahedral (HOH) high-index-faceted Cu nanoparticles were integrated with a porous Ag foam to construct Cu/Ag tandem catalysts for CO2 electroreduction. The C2+ selectivity follows the order HOH Cu/Ag > THH Cu/Ag > non-facet-controlled Cu/Ag, with HOH Cu/Ag achieving the highest ethylene Faradaic efficiency of 60.37%. In situ spectroscopic measurements using HOH Cu/Ag as a representative high-index-faceted catalyst indicate the formation of abundant adsorbed CO and possible CO-derived coupling intermediates within the potential range associated with pronounced ethylene production. Stability measurements further show that the morphology and catalytic selectivity are largely retained under moderate operating conditions, whereas more negative potentials induce surface roughening and gradual performance decay. This work provides a platform for investigating morphology-dependent selectivity in high-index-faceted Cu catalysts during CO2 electroreduction.
✓ 已验证
产品关联
DOI
高影响因子
Chemistry-An Asian Journal
·
2026
·Vol. 21
·期 17
·e70895
·
IF 3.2
Zhe Wang,Tang Tang,Jianpei Feng,Haihang Tong,Chun Hong Mak,Adel Zrelli,Alvaro Muñoz-Castro,Ji-Jung Kai,Carol Sze Ki Lin,Patrick H.-L. Sit,Hsien-Yi Hsu
Metal halide perovskites have exhibited considerable potential for solar-driven photocatalytic CO 2 reduction, yet their practical application is largely hindered by lead toxicity and severe charge recombination. In this work, we report the synthesis and screening of lead-free halide double perovskite Cs 2 AgBiX 6 (CABX, X = Cl, Br, I) nanocrystals via an antisolvent technique, followed by the construction of Cs 2 AgBiX 6 @WS 2 (CABBWS) composites with varying WS 2 contents (25, 50, 75 mol%). Structural and interfacial characterizations confirm the intimate contact between CABB particles and WS 2 nanosheets, while photophysical and photoelectrochemical (PEC) analyses demonstrate the optimal CABBWS50 with superior charge separation properties. The CABB-WS 2 intimate interface enhances charge transport by reducing activation energy, as evidenced by temperature-dependent TRPL measurements. The optimal CABBWS50 achieves a CO evolution rate of 13.65 µmol g − 1 h − 1 under visible-light irradiation ( λ > 420 nm), approximately 3.7 times higher than pristine CABB. This work provides comprehensive insights into the design of high-performance lead-free perovskite photocatalysts via rational halogen engineering and interfacial regulation, offering a promising strategy for solar fuel production toward carbon neutrality.
✓ 已验证
产品关联
DOI
高影响因子
AICHE JOURNAL
·
2023
·
IF 3.7
Jiajin Huang,Liang Yu,Qichen Fan,Jinze Yao,Yongsheng Huang,Haoyuan Luo,Baoyu Liu,Hao Wang,Qibin Xia
The purification of gaseous olefins, such as C 2 H 4 and C 3 H 6 , requires the efficient removal of trace CO 2 impurities. However, the development of ideal adsorbents with high CO 2 /olefin selectivity has remained a challenge. In this study, we synthesized a novel adsorbent, denoted as PEI/DEA@FS, by modifying fumed silica (FS) with a combination of polyethylenimine (PEI) and diethanolamine (DEA). At 298 K and 0.0004 bar, PEI/DEA@FS presented the highest CO 2 adsorption capacity among previously studied adsorbents, with a value of 2.12 mmol/g. Notably, PEI/DEA@FS demonstrated very high ideal adsorption solution theory selectivity for CO 2 /C 2 H 4 (>10 10 ) and CO 2 /C 3 H 6 (>10 7 ) at 298 K and 0.01 bar. Breakthrough experiments revealed its excellent separation performance, producing olefins (C 2 H 4 and C 3 H 6 ) with ultra-high purity (>99.9%) from a CO 2 /olefin (1/99) mixture. Moreover, PEI/DEA@FS exhibited outstanding stability over 20 adsorption and desorption cycles, and its CO 2 adsorption performance remained almost unchanged under 75% relative humidity in the feed stream.
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2026
·
IF 3.9
Fengting Yao,Zhixu Yun,Ziheng Li,Xuehua Ruan,Yan Dai,Xiaoming Yan,Xiaobin Jiang,Wenji Zheng,Gaohong He
Abstract Metal-organic framework (MOF)-based mixed-matrix membranes (MMMs) are promising for CO2 separation but remain limited by poor filler–polymer compatibility and compromised molecular sieving at high filler loadings. Herein, we developed a hydrogen-bond-mediated molecular interfacial engineering strategy by constructing complementary donor–acceptor hydrogen-bond networks between NH2-ZIF-8 and a carboxylated polyimide (COOH-PI), enabling the synergistic regulation of interfacial compatibility and the MOF pore microenvironment. The hydrogen-bonding network strengthened interfacial adhesion, suppressed nonselective defects, enhanced CO2 affinity, and optimized the ultramicroporous structure, while amination narrowed the MOF pore aperture to improve molecular sieving. The MMM containing 25 wt.% NH2-ZIF-8 with 15% amination exhibited excellent interfacial integrity and long-term operational stability, while its CO2/CH4 and CO2/N2 separation performances lie above both the 2008 Robeson upper bound and the revised 2019 upper bound reported by Neil B. McKeown et al. This strategy provides a general approach for designing high-performance CO2 separation MMMs.
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2023
·
IF 16.5
Hangjie Li,Yuehua Xiao,Jiale Xiao,Kai Fan,Bingkuan Li,Xiaolong Li,Liang Wang,Feng-Shou Xiao
Supported Cu catalysts are widely studied for the hydrogenation of CO 2 to dimethyl ether (DME). However, they suffer from insufficient durability and DME selectivity. Herein, we overcome these issues by modulating the gallium species and hydrophobic methyl groups to obtain a silica-supported copper catalyst , achieving a Cu/Ga-SiO 2 -Me catalyst with significantly improved DME selectivity and catalyst durability. Characterizations of the catalysts showed that the gallium species electronically modulated the Cu nanoparticles , resulting in abundant Cu δ + species in the catalyst, which minimized the reverse water-gas shift reaction and thus reduced CO selectivity. In addition, the methyl groups contributed to the rapid removal of water from the catalyst surface, which hindered Cu sintering and accelerated catalysis. Consequently, the Cu/Ga-SiO 2 -20Me exhibited a CO 2 conversion of 9.7%, selectivities of DME and methanol of 59.3% and 28.4%, and CO selectivity of only 11.3%. The strategy used in this study may provide rational guidance for improving current industrial catalysts.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Ganghua Zhou,Longyun Zhang,Yu Xia,Hangmin Xu,Weiqin Yin,Shengsen Wang,Jianjian Yi,Xingwang Zhu,Xin Ning,Xiaozhi Wang
Solar-driven conversion of CO 2 into high-value-added chemicals is considered as one of the effective strategies to address global climate change. However, the sluggish charge separation kinetics and poor product selectivity remain the two major bottlenecks restricting photocatalytic CO 2 conversion. Herein, we developed an anatase surface modified atomically dispersed Cu (Cu anchored on N-doped carbon skeleton) photocatalyst (TiO 2 /Cu 1 NC) based on a “reflux + calcination” method for CO 2 photoreduction. Under full spectral illumination, the as-synthesized TiO 2 /Cu 1 NC displayed a brilliant CO production rate of 2.59 μmol h −1 (mass of photocatalyst: 5 mg), high selectivity (∼98.5%), and excellent durability using [Ru(bpy) 3 ]Cl 2 ·6H 2 O as the photosensitizer and triethanolamine as an electron donor. Experiments and density functionalized theory calculations synergistically confirm that the surface-constructed atomically dispersed Cu 1 NC active sites can accelerate the separation and transfer of photogenerated charge carriers, optimize CO 2 adsorption and activation, reduce the formation energy barrier of the key intermediate *COOH during the CO 2 RR process, and thus enhance the activity and selectivity of CO 2 RR. This work provides new insights into the surface engineering of atomically dispersed active sites to improve the activity and CO selectivity of CO 2 photoreduction.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Ying Zhang,Linlin Zang,Shuting Zhao,Weipeng Cheng,Long Zhang,Liguo Sun
Covalent organic frameworks (COFs) have great potential for photocatalytic CO 2 reduction, owing to their adjustable structures, porous characteristics, and highly ordered nature. However, poor light absorption, fast recombination of photogenerated electron-hole pairs, and suboptimal coordination conditions have contributed to the hindered efficiency and selectivity observed in photocatalytic CO 2 reduction processes. In this work, the integration of bromine (Br) atoms into COFs was achieved through the synthesis process involving nickel (II) tetraaminophthalocyanine (NiTAPc) and 3,6-dibromopyromellitic dianhydride (BPMDA) using a solvothermal approach. The coupling of a porous framework structure alongside the incorporation of Br atoms yields a significant enhancement in photoelectric properties compared to bromine-free COFs. Meanwhile, X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) calculations revealed that the introduction of Br atoms can facilitate the adjustment of the electron configuration around the phthalocyanine unit and diminish the required energy for the photocatalytic reaction. When subjected to visible light irradiation, the NiTAPc-BPMDA COF showcased a CO yield of 148.25 μmol g −1 over a 5-hour period, accompanied by an impressive selectivity of 98%. This work highlights the collaborative influence of phthalocyanines and Br atoms within COF-based photocatalysts, offering an alternative approach for designing and constructing high-performance photocatalysts with elevated yield and selectivity. The synergistic role of phthalocyanines and Br atoms within the COF-based photocatalysts provides an alternative strategy for photocatalysts with high yield and selectivity in the future.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Lang Pei,Xusheng Wang,Heng Zhu,He Yu,Sateesh Bandaru,Shicheng Yan,Zhigang Zou
Photothermal catalysis, which combines light promotion and thermal activation, is a promising approach for converting CO2 into fuels. However, the development of photothermal catalysts with effective light-to-heat conversion, strong charge transfer ability, and suitable active sites remains a challenge. Herein, the photothermal effect- and interfacial N–Ni/Ta–O bond-modulated heterostructure composed of oxygen vacancy-rich NiOx and Ta3N5 was rationally fabricated for efficient photothermal catalytic CO2 reduction. Beyond the charge separation capability conferred by the NiOx/Ta3N5 heterojunction, we observed that the N–Ni and Ta–O bonds linking NiOx and Ta3N5 form a spatial charge transfer channel, which enhances the interfacial electron transfer. Additionally, the presence of surface oxygen vacancies in NiOx induced nonradiative relaxation, resulting in a pronounced photothermal effect that locally heated the catalyst and accelerated the reaction kinetically. Leveraging these favorable factors, the NiOx/Ta3N5 hybrids exhibit remarkably elevated activity (≈32.3 μmol·g–1·h–1) in the conversion of CO2 to CH4 with near-unity selectivity, surpassing the performance of bare Ta3N5 by over 14 times. This study unveils the synergistic effect of photothermal and interfacial chemical bonds in the photothermal–photocatalytic heterojunction system, offering a novel approach to enhance the reaction kinetics of various catalysts.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
FUEL
·
2023
·
IF 7.4
Anbang He,Yong Yang,Shuhui Tao,Xubing Zhou,An Wu,Qian Zhang,Changyuan Tao,Jun Du
Co 3 O 4 -based catalysts emerged as promising candidates for electrocatalytic CO 2 reduction reaction (eCO 2 RR), while the unclear active sites and poor stability are challenging for the application of Co 3 O 4 as an electrocatalyst. Here, we developed a feasible method to in situ encapsulate Co 3 O 4 nanoparticles (NPs) into self-grown CNTs . Co 3 O 4 NPs were elaborately controlled to terminate with the occupation Co 2+ Th /Co 3+ Oh sites (with Co 2+ and Co 3+ in the center of tetrahedral/octahedral cells). The well-dispersed Co atoms derived from ZIF-67 catalyzed the in situ assembly of CNTs, allowing controlled oxidation and growth into Co 3 O 4 nanoparticles spatially confined by CNTs, resulting in Co 3 O 4 highly-dispersed into hollow CNTs and well-protected. The enhanced electrocatalytic performance of Co 2+ Th was revealed with an onset potential of −0.24 V, and the CO production rate (131 μmol/s·g·cm 2 , −0.85 V vs. RHE) on Th-Co 3 O 4 /CNTs (exposed with Co 2+ Th sites) is 3.1 times of that on Oh-Co 3 O 4 /CNTs (exposed with Co 3+ Oh sites). DFT calculations demonstrated a significant reduction in the rate-limiting activation barrier of CO 2 , and Co 2+ Th was proved to be more active than Co 3+ Oh with elongated *CO-OH bonds. In situ ATR-SEIRAS confirmed that the enhanced CO 2 adsorption and rapid formation of *COOH on Th-Co 3 O 4 /CNTs were key factors leading to efficient CO production. This work introduced a clear understanding of the eCO 2 RR performance of Co 2+ Th /Co 3+ Oh sites, along with a feasible approach for catalyst construction and protection.
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Yi Liu,Shuangjiang Li,Manoj Pudukudy,Li Lin,Huigui Yang,Mengrui Li,Shaoyun Shan,Tianding Hu,Yunfei Zhi
Constructing green and efficient porous material platforms for carbon dioxide (CO 2 ) adsorption and chemical conversion can effectively solve a series of environmental problems caused by the greenhouse effect. Herein, four melamine-based polymer networks PANs (PAN-P, PAN-PY, PAN-PZ, and PAN-IM) with abundant N sites and hydrogen bond donor (HBD) groups were synthesized by simple polymerization. The chemical structure of PANs was determined by various characterizations, and then the CO 2 uptake of PANs and their catalytic activity for the cycloaddition of CO 2 with epoxides were investigated. Among them, PAN-P has the largest CO 2 adsorption capacity, reaching values of 73.5 cm 3 /g at 273 K. Meanwhile, PAN-IM exhibits the best catalytic activity with 93 % yield and 99 % selectivity under metal-, halogen-, solvent-, and cocatalyst-free conditions (120 ◦C, 1.0 MPa CO 2 , 8 h), which mainly attribute to the multi-site synergistic activation of the imidazole heterocycle. In addition, PAN-IM also has satisfactory activity to various epoxides and exhibited good recyclability. Density functional theory (DFT) and FT-IR analysis were used to further reveal the interaction of PANs towards CO 2 and epoxides. Finally, a possible mechanism was suggested, including activation of CO 2 and epoxide, ring-opening of epoxide, insertion of CO 2 and ring-closing to form cyclic carbonate. The research in this paper will provide a reference for the development of a green and efficient CO 2 adsorption conversion platform.
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2023
·
IF 7.4
Tingman Zhao,Bo Feng,Jiada Du,Shengdao Shan,Yun Shi
Low-temperature NH 3 -SCR of NO x technology was recognized as a promising way to control NO x emissions from industrial kilns at low temperatures. Except for SO 2 and H 2 O, lots of CO 2 exist in the flue gas of industrial kilns. However, there are few researches on the effects of CO 2 on the low-temperature NH 3 -SCR activity. To investigate the effects of CO 2 on the low-temperature NH 3 -SCR performance and mechanism of CeO x -biochar catalyst, a series of experiments employed. The results showed that the presence of CO 2 had an obvious inhibitory effect on the NH 3 -SCR performance of CeO x -biochar 0.6 at 150 °C. There was competitive adsorption between CO 2 and NO on the surface of CeO x -biochar 0.6 . CO 2 was mainly adsorbed on CeO 2 , which hindered the oxidation of NO and the adsorption of NO x on the catalyst surface. Meanwhile, although the presence of CO 2 could improve NH 3 adsorption capacity of CeO x -biochar 0.6 due to the formation of NH 4 HCO 3 and (NH 4 ) 2 CO 3 , the existence of carbonates and bicarbonates blocked the formation of active intermediates NH 4 NO 2 and NH 2 NO for NH 3 -SCR reaction. As a result, the NO x conversion of CeO x -biochar 0.6 was dropped from 96.9% to 40.8% at 200 °C. In view of the bicarbonate and carbonate species was unstable at high temperatures, the inhibitory effect of CO 2 on NH 3 -SCR reaction was gradually weakened with the increase of reaction temperature. The NH 3 -SCR activity of CeO x -biochar 0.6 was seldom affected by CO 2 at 300 °C. Finally, a CO 2 poisoning mechanism for NO x removal by NH 3 -SCR at low temperature was proposed.
✓ 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）