Inorganic Chemistry Frontiers
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2025
·
IF 6.4
Rui Lu,Aimin Yao,Yali Dai,Haijiao Yin,Chengqi Li,Yuanxin Du,Manzhou Zhu
Developing heterogeneous nanocatalyst with well-defined structure and excellent reactivity and stability is vital for understanding catalytic mechanism and practical industrial application. Herein, we report the construction of atomically precise metal nanocluster sandwich heterojunction (MIL-125-NH2-Au25(L-Cys)18/g-C3N4, M-A/C for short). Compared with the binary counterparts, the M-A/C efficiently and selectively photocatalyzes CO2 reduction to methanol under visible light irradiation with remarkably enhanced activity and stability, due to the protective shell. Moreover, the ternary M-A/C heterojunction not only broadens light absorption region, strengthens CO2 adsorption, but also expands interface charge transfer channel, benefiting for photocatalytic performance. Additionally, the integrating of precise structure and in situ spectrometry unveils the evolution from CO2 to CH3OH. This work opens a promising avenue to design highly-efficient and robust atomically precise metal cluster-based heterojunction catalyst.
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Molecular Catalysis
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2025
·
IF 4.9
Hui Kang,Quan Shao,Luming Li,Yanlin Zhang,Xin Xiao,Yuefeng Liu
The gas-inducing strategy has proven highly effective in constructing high-density oxide interfaces. In this study, we utilized CO 2 hydrogenation reaction to induce the spontaneous dispersion of In 2 O 3 species on the surface of TiO 2 , forming numerous InO x /TiO 2 interfaces. The 2 %In 2 O 3 /TiO 2 catalyst demonstrated a 33-fold enhancement in reverse water-gas shift reaction (RWGS) performance after dispersion. Multi-technique characterization revealed that H 2 in the reactants reduced In 2 O 3 to partially reduced states (In +(3-x) ), which were more prone to migration. The spontaneous dispersion was not solely driven by the strong interaction (anchoring) ability of the support for In 2 O 3 species. Further mechanistic studies showed that the high-density InO x /TiO 2 interface formed via spontaneous dispersion significantly promoted the formation of formate species during CO 2 hydrogenation, which decomposed into CO at lower temperatures (297 °C), thereby improving catalytic performance. This work highlights the potential of atmosphere-induced structural evolution in catalysis, underscoring the importance of a comprehensive analysis of the activation, migration, and anchoring mechanisms, as well as the catalytic promotion principles of the induced structure.
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Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Yulan Xu,Minxian Wu,Xianxian Zhang,Zhihui Zhang,Yanli Chen,Haiguang Gao,Huazhang Guo,Wenchang Wang,Naotoshi Mitsuzaki,Zhidong Chen
Ga-Sn liquid metal catalysts exhibit high activity in the electrochemical conversion of CO 2 to formic acid. However, achieving high current densities for industrial-scale production is still challenging. A facile one-step electrodeposition method for preparing Ga-Sn thin films on metal foam substrates was proposed. A deep eutectic solvent consisting of choline chloride and urea, which is known as Reline, was used as the electrolyte solvent. The electrochemical behaviors of Sn(II)/Sn(0) and Ga(III)/Ga(0) in Reline were studied on a Pt rotating disk electrode. The diffusion coefficient and exchange current density of Sn(II) and Ga(III) in this electrolyte were determined by the Koutecký-Levich equation. Ga91.6Sn8.4 thin liquid film was electrodeposited on a copper foam substrate and used as the catalytic electrode for electrochemical reduction of CO 2 in a CO 2 -saturated 0.1 M KHCO 3 solution, and a high Faradaic efficiency (90 %) for HCOOH was achieved. Density functional theory (DFT) simulations were conducted to gain deeper insight into the role of the alloy in the CO 2 reduction reaction (CO 2 RR). The results indicate that the incorporation of Sn into the alloy not only introduces additional active sites for *OCHO adsorption but also facilitates the conversion of *COOH intermediates to formate.
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ENVIRONMENTAL RESEARCH
·
2025
·
IF 7.7
Dong Liu,Zelu Zhou,Zhitao Han,Mengjing Zhang,Aicheng Song,Xi Wu,Xiao Yang,Dong Ma
In recent years, significant attention has been drawn to the advancement of high-performance solid acid catalysts, which enhance the CO 2 desorption efficiency and concurrently lower energy requirements. Although solid acid catalysts show promise in reducing regeneration energy for amine-based CO 2 capture, achieving an optimal balance between activity, cost, and stability remains a major challenge. Herein a series of solid acid catalysts were prepared by modifying attapulgite (ATP) with various CuO x loading, and the effect of Cu modification on CO 2 desorption performance was compared systematically. The results showed that CO 2 desorption performance of the as-prepared catalysts was in an order of 2/1-CuO x /ATP >1/1-CuO x /ATP >3/1-CuO x /ATP > CuO > ATP. The CO 2 desorption capacity and rate were increased by 194 % and 205 %, respectively, the relative heat duty could be reduced by about 64.5 % by using 2/1-CuO x /ATP to regenerate the rich MEA solution. ATR-FTIR technique was employed to confirm the catalytic effect and a possible catalytic CO 2 desorption mechanism was suggested. Additionally, the catalyst maintained 81 % of its initial CO 2 desorption capacity after seven consecutive absorption-desorption cycles, demonstrating excellent recoverability. This study provides a practical strategy for utilizing efficient, affordable and environmentally benign solid acid catalysts for CO 2 desorption, thereby advancing energy-efficient CO 2 capture technology.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Kaiwen Ma,Jian Sun,Rongyue Sun,Chuanwen Zhao
Lately, Ca-based sorbents with a core–shell structure have been effectively produced to augment the sorbent’s capabilities. However, modifying the pristine core of Ca-based pellets with a core–shell structure notably influences the performance of the synthesized sorbent, and research in this domain remains scarce. Here, two categories of Al-stabilized, Ca-based pristine cores were produced using Ca(OH) 2 mixed with Al-based stabilizer precursors of insoluble aluminum oxide and soluble aluminum nitrate, respectively, through the extrusion-spheronization technique. Due to the impact of mechanical extrusion, soluble aluminum nitrate can accumulate in-homogeneously in the Ca-based pristine core, leading to its expansion and rupture during the high-temperature calcination stage because of the decomposition of aluminum nitrate. The oxide-form aluminum stabilizer precursor can be uniformly distributed throughout the Ca-based pristine core pellets, demonstrating notably superior cyclic CO 2 sorption capability and mechanical strength. The Al-fortified, core–shell structured Ca-based sorbent pellets demonstrated a peak CaO carbonation conversion rate of 54.8 % after 100 cycles when the Ca:Al molar ratio was precisely set to 85:15, which is about 2.1 times higher compared to the core–shell Ca-based sorbent pellets composed of a pure CaO core. This is primarily due to the formation of an evenly distributed inert Ca 12 Al 14 O 33 within the pristine core, which effectively reduces high-temperature sintering. Hence, core–shell Ca-based sorbent pellet assembled with an Al-stabilized pristine core, could be a promising candidate for application in the CaL process for CO 2 capture.
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Environmental Science-Nano
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2025
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IF 5.1
Jiang Liu,Longyu Wang,Wenzhao Sun,Runhu Li,Yuanshui Zhen,Shiyuan Guo,Bo Wang,Xingguang Xu
The escalating global demand for energy and the urgent need to mitigate climate change have spurred the development of next generation carbon capture utilization and storage (CCUS) techniques. This study introduces novel amine-functionalized silica nanoparticles (PEI@SiO2-KH550 NPs) as a high-performance CO2 carrier for CCUS applications. The nanoparticles were synthesized via a facile two-step modification process: grafting 3-aminopropyltriethoxysilane (KH550) onto silica nanoparticles, followed by coating with polyethyleneimine (PEI). This design significantly enhances CO2 absorption capacity by enriching the surface amine groups, so more CO2 will be carried into the target formation, interact with the oil and be stored underground. The resultant nanofluid (0.8 wt% concentration) demonstrated exceptional CO2 uptake (∼100 cm3 under ambient conditions in 40 minutes) and dispersion stability (zeta potential: +38.21 mV). Rheological analyses revealed its shear-thinning behavior, ensuring injectivity in porous media. Remarkably, CO2-saturated nanofluid reduced the dynamic interfacial tension (IFT) between crude oil and water from 19.24 mN m−1 to 7.82 mN m−1, primarily attributed to nanoparticle adsorption at the oil–water interface and in situ generation of surface-active carbamates. In addition, the pressure drop experiment revealed that the presence of PEI@SiO2-KH550 in the aqueous phase could significantly promote the CO2 diffusion rate and facilitate the mass transfer. Besides, molecular dynamics simulations demonstrated that PEI@SiO2-KH550 enhanced the CO2 saturated-nanofluid/crude oil interaction through impacting the interfacial energy (IFE), the radial distribution function (RDF) of light and heavy oil components, the interface thickness and the CO2 diffusion coefficient. Core flooding experiments validated the dual effectiveness of the developed nanofluid, achieving 79.8% oil recovery (10% higher than the carbonated water) and 48.6% CO2 sequestration rate (16.7% higher than carbonated water). The innovation lies in the nanoparticles' scalable synthesis, dual functionality (CO2 capture and interfacial modification), and compatibility with harsh reservoir conditions. This work may provide enlightening insights for integrating CO2-enhanced oil recovery (EOR) with CO2 geological storage, advancing next-generation CCUS technology.
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Korean Journal of Materials Research
·
2025
·Vol. 35
·期 8
·352-365
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IF 0.3
Haixia Wang,Yilei Sun,Yao Liu,Kunjie Li,Zeda Meng,Won-Chun Oh
The catalyst materials 0N-Cu-MOF, 1N-Cu-MOF, and 2N-Cu-MOF were successfully synthesized usinga solvothermal method, and using different concentrations of nitrogen-modified Cu organic frameworks (xN-Cu-MOF). Characterizations using X-ray diffraction (XRD), scanning electron microscopy (SEM), fourier transform infrared (FT-IR) spectroscopy, X-ray photoelectron spectroscopy (XPS), and Brunauer-Emmett-Teller (BET) surface area analysis showed that 1N-Cu-MOF had the largest SSA and pore size among the three materials synthesized. 1N-Cu-MOF exhibited the largest pore size and specific surface area among the three materials, which had a decisive effect on CO2 reduction. In addition, stability and CO2 reduction reaction (CO2RR) activity were evaluated by linear sweep voltmeter, cyclic voltmeter, electrochemical impedance spectroscopy, and time flow tests. Faradaic efficiency (FE) was determined by product analysis. Among the three catalyst materials, 1N-Cu-MOF showed the best catalytic performance at 50 mA·cm-2 (maximum current density). The charge transfer resistance was 8.23 Ω, the average current density was 19.9 mA·cm-2, and the FE of methane (CH4) production showed a high efficiency of 70.45 % when tested for 12 h at an overpotential of -0.35 V (to-RHE).
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Nanomaterials
·
2025
·Vol. 16
·期 1
·35
·
IF 4.3
Wenjing Wu,Zichao Yang,Min Zhang,Zhongjie Guan,Jianjun Yang
Photocatalytic reduction of carbon dioxide is a very effective strategy to address the energy crisis and greenhouse effect. TiO2is a widely used semiconductor photocatalyst, which has excellent catalytic activity, excellent chemical stability and low toxicity. Nevertheless, TiO2still has some inherent limitations, such as: wide band gap, high carrier recombination rate, and low adsorption activation ability for carbon dioxide. These drawbacks severely restrict its further application in the photocatalytic reduction of CO2. In this study, cotton-like blue C/TiO2NTs are successfully synthesized through the in situ growth of TiO2nanotubes on the MIL-125(Ti)-derived C/TiO2precursor. The experimental results revealed that the CO production rate of the cotton-like blue C/TiO2NTs was 1.84 times that of C/TiO2and 3.78 times that of TiO2nanotubes. These results clearly demonstrate that the cotton-like blue C/TiO2NTs exhibit a broad spectral response, a large specific surface area, and an abundance of oxygen vacancies. This research provides new insights into the design of titanium dioxide-based photocatalytic materials and opens up a promising avenue for enhancing the performance of titanium dioxide in the photocatalytic reduction of carbon dioxide.
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ENERGY & FUELS
·
2025
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IF 5.3
Qiulin Ye,Dongdong Wang,Jiabao Lv,Minghui Tang,Angjian Wu,Yaqi Peng,Shengyong Lu
The electrocatalytic CO2 conversion offers a sustainable pathway for generating ecofriendly chemicals and fuels while simultaneously enabling the storage of intermittent renewable energy. Herein, CuPd bimetallic catalysts were specifically designed through displacement reaction, with a magnetron sputtering Cu film as a substrate. The optimized CuPd catalyst achieved an ethylene Faradaic efficiency (FE) of 51.07% and a C2+ FE of 82.18% at a 200 mA/cm2 current density. In situ Raman spectroscopy indicates that the CuPd electrode exhibited a high local surface pH during the CO2 reduction reaction, which was favorable for C–C coupling. The observation of the *OCCOH intermediate by in situ FTIR, combined with density functional theory calculations, confirms that the CuPd surface promotes C–C coupling instead of direct hydrogenation. This mechanistic insight explains why the addition of Pd enhances the selectivity for C2+ products.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2021
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IF 3.764
Xiaonan Zhao,Wei Liu,Xiufeng Liu,Baoquan Zhang
Mixed matrix membranes (MMMs) are challenged by the poor compatibility between fillers and a polymer matrix that leads to the weakened performance for gas separation. The surface modification of fillers with aminosilane should be an effective approach to improve their compatibility within the polymer matrix. 3-(2-Aminoethylamino)propyl-dimethoxymethylsilane (APDS) was used as a silane coupling agent for modification of sheet-like silicoaluminophosphate-34 (SAPO-34) crystal grains, and novel MMMs were fabricated by incorporating APDS-modified SAPO-34 crystal grains into a Pebax MH 1657 polymer. Based on characterization using scanning electron microscopy (SEM), X-ray diffraction (XRD), Fourier transform infrared (FTIR) spectroscopy, and mechanical tests, the incorporation of an APDS-modified SAPO-34 into Pebax matrix led to much enhanced interfacial adhesion within the MMM. In addition, the effect of the filler content in the MMM on the separation performance of a CO2/CH4 gas mixture and pure gases (CO2 and CH4) was investigated. Compared with available Pebax-based MMMs in the literature, the prepared MMM containing 8 wt % APDS-modified SAPO-34 exhibited the satisfactory CO2 permeability of ca. 137 Barrer and the highest selectivity of 34.7 for the CO2/CH4 gas mixture. It was believed that the excellent separation performance and good stability of the prepared MMM in this study should be due to the good interfacial compatibility of APDS–SAPO-34 fillers together with their strong affinity for CO2 within the MMM.
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Small
·
2022
·Vol. 18
·期 45
·2204490
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IF 15.153
Bing Han,Qinghe Li,Xunzhu Jiang,Yalin Guo,Qike Jiang,Yang Su,Lin Li,Botao Qiao
The switch of CO 2 hydrogenation selectivity from CH 4 to CO over TiO 2 supported Rh catalysts is accomplished via selective encapsulation of Rh nanoparticles while exposing Rh single atoms by high-temperature reduction (HTR) according to their different strong metal-support interaction (SMSI) occurrence conditions, which can be reversed by subsequent oxidation treatment.
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ACTA PHYSICO-CHIMICA SINICA
·
2023
·
IF 10.9
Haoyu Sun,Dun Li,Yuanyuan Min,Yingying Wang,Yanyun Ma,Yiqun Zheng,Hongwen Huang
In recent years, Cu-based multi-metallic nanocrystals with controlled elemental distributions have been extensively studied for potential applications as electrocatalysts for CO 2 reduction reaction (CO 2 RR). Modifying Cu electrocatalysts with secondary or additional metals offers a viable approach to manipulate the overall d -band structure which would cause the shift in the d -band center. Such manipulation can affect the surface affinity of Cu towards key intermediates and thus the following catalytic pathway. Apart from endeavors to adjust the electronic structure, morphological engineering provides effective avenues to enhance the electrocatalytic performance of CO 2 RR. In contrast to quasi-spherical particles with irregular shapes, a 3D-assembled porous structure utilizing 2D nanosheets as building blocks offers advantages such as maximizing surface atom exposure and creating numerous diffusion channels and reactive sites for intermediates formed during catalysis. Yet, it is technique challenging to construct such type of nanoarchitecture via a rationally-design synthetic routes and traditional stepwise self-assembling strategy is time-consuming and lack of versatile control over the structural parameters of resulting products. Therefore, it holds significant value to develop a synthesis method capable of yielding high-purity formations of unique nanostructures. These structures should possess accurately controlled elemental compositions and electronic configurations, and establish a potential correlation between structural benefits and enhanced electrochemical performance in CO 2 RR. Herein, we report the controlled synthesis of palladium-copper-silver (Pd-Cu-Ag) nanocrystals with rationally-designed two-dimensional (2D)-three-dimensional (3D) hybrid architectures and validated with the promising use for electrochemical CO 2 reduction (CO 2 RR). The synthetic procedure includes the conversion of Au@Cu x O nanospheres into CuAg hierarchical nanoflowers (HNFs), as directed by the capping agent octadecyltrimethyl ammonium chloride. Interestingly, the nanosheets are formed in situ as the building block. Following galvanic replacement reaction between CuAg HNFs and Na 2 PdCl 4 removes Ag and Cu, introduces zero-valent Pd, and creates abundant pores on the nanosheets. These CuAg-based products are tested as CO 2 RR electrocatalysts, in which the Pd 0.7 Cu 40.0 Ag 59.7 PHNFs displayed the optimized performance in terms of C 2+ products selectivity (69.5%) and C 2+ partial current density (−349.1 mA·cm −2 ). As revealed by density functional theory (DFT) simulations, PdAgCu surface has distinct electronic property, which lower the reaction barrier for C-C coupling, protruding the exceptional advantage of the Pd doping towards CuAg electrocatalysts for CO 2 reduction. The present study offers a straightforward approach to fabricate hierarchical multi-metallic nanostructures with the porous nanosheet as building block, and validates its structural advantage in electrocatalysis, shedding light on the rational design of efficient CO 2 RR catalyst. Download: Download high-res image (72KB) Download: Download full-size image
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