APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Xi Liu,Xueting Zhao,Zhiwen Lu,Kai Chen,Jiyuan Gao,Huibing Wang,Junxiang Chen,Zhenhai Wen
Amorphous electrocatalysts, unconstrained by crystalline order, offer a versatile landscape of active sites that promote enhanced reactivity and structural adaptability. When fused with the compositional complexity of high-entropy materials, this disordered architecture yields enhanced electronic interactions and catalytic adaptability. In this work, we design a self-supporting amorphous high-entropy oxide (a-HEO) electrode by in-situ growth of FeCoNiMnMo-based nanosheets on nickel foam (a-FeCoNiMnMoO/NF). Electrochemical activation triggers a self-reconstruction process, yielding oxyhydroxide species embedded with oxygen vacancies that collectively enhance electron conductivity and catalytic performance for the alkaline methanol oxidation reaction (MOR). Machine learning potential-based simulations demonstrate that the amorphous oxyhydroxide layer offers a diverse array of catalytic sites, fine-tunes the electronic structure, and optimizes intermediates adsorption, thus enhancing the reaction dynamics of methanol oxidation. When employed in a hybrid acid/alkali flow electrolyzer, the system operates at just 0.54 V to reach 10 mA cm −2 , enabling over 300 h of continuous, CO 2 -free production of hydrogen and formate, demonstrating a durable and energy-saving strategy for sustainable fuel and chemical generation. This study highlights the compelling synergy between structural disorder and elemental complexity, charting a promising course toward low-energy, carbon-neutral methanol reforming and sustainable hydrogen production.
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Journal of the American Chemical Society
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2025
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IF 15.6
Hang Zhang,Zhiwen Jiang,Changjiang Hu,Pengfei Zheng,Jun Ma
The hydro/dicarboxylation of ethylene (C2H4) feedstock with CO2 to produce high-value carboxylic acids is an industrially relevant yet challenging reaction due to their extremely low reactivities. Herein, we present an effective strategy to synthesize propionic acid and succinic acid from a mixture of CO2 and C2H4 catalyzed by high-energy water radiolysis. The process involves the generation of CO2 radical anions via the barrierless attachment of hydrated electrons to CO2, facilitating an ambient, continuous carboxylation of C2H4 with an efficiency of 81.4%. Utilizing easily available electron beam irradiation, we achieved a combined production rate of 0.34 mmol L–1 min–1 for carboxylic acids, which is unattainable by the existing methods. Notably, product selectivity between hydro- and dicarboxylation was dose-rate/beam intensity-dependent: high-dose-rate irradiation favored succinic acid formation with a proportional yield of up to 65.4%, while milder conditions resulted in an 85.1% yield of propionic acid. We suggested that the simplicity and efficiency of the present carboxylation approach promote circular carbon in the sustainable chemical industry.
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Molecular Catalysis
·
2024
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IF 3.9
Pengcheng Wang,Qingqing Jiang,XingYu Li,Xuedong Wang,Juncheng Hu
Generally, researchers focus on the regulation of metal sites rather than surrounding nonmetals in photothermal CO 2 hydrogenation reaction. Herein, concerning the role of non-metallic N species, a series of Co/NC-T catalysts have been fabricated via high-temperature pyrolysis of Zeolitic Imidazolate Frameworks-67. The CO 2 conversion rate shows a consistent tendency with the ratio of graphitized-N species while the product selectivity is closely related to the coordination state of Co-N x species. Co/NC-800 catalyst achieves high CO 2 conversion rate of 758 mmol g cat -1 h -1 with CH 4 selectivity of 99.6 %. After adding extra graphitized-N species, the CO 2 conversion rate could further enhance to 80.2 % for N-Co/NC-2. The role of N species in photothermal CO 2 hydrogenation reaction has been investigated in details, providing new insights for the design of metal organic frameworks derived metal/N-doped carbon catalysts.
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MACROMOLECULAR CHEMISTRY AND PHYSICS
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2025
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IF 2.7
Siriguleng Bao,Yong Sheng Bao,Agula Bao
Lignin has a high carbon content, but the production of porous carbon materials from it is challenging because of its complex structure and stable physicochemical properties. In this study, nitrogen-doped porous carbon materials are prepared by impregnating lignin with urea, using potassium hydroxide (KOH) as an activator. The physicochemical properties of the samples are investigated using various characterization methods. The results showed that the CO 2 adsorption capacity of the sample LUN-10-7, which has a urea solution concentration of 10% and an immersion time of 7 days, is 3.80 mmol g −1 at 1 bar and 298 K. The characterization results indicated that the abundant pore structure and excellent surface chemistry enhanced the sample's CO 2 adsorption performance. Additionally, the sample demonstrated high CO 2 /N 2 selectivity and cyclic stability, making it suitable for practical applications as an adsorbent.
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LANGMUIR
·
2025
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IF 3.9
Yongtao Zhang,Zaizheng Jiang,Zhihe Xin,Qingqi Dong,Fei Wang
Traditional coal burning emits a large amount of pollutants, including sulfur dioxide (SO2), nitrogen oxides, and carbon dioxide (CO2), severely contaminating the environment and exacerbating global warming. In contrast, integrated gasification combined cycle (IGCC) technology, with highly efficient and clean characteristics, significantly reduces pollutant emissions and has a positive impact on environmental protection. It is a simple and effective method to obtain hydrogen (H2) by purifying IGCC fuel gas with the main components of H2 and CO2. Thermodynamic promoter tetra-n-butyl ammonium bromide (TBAB) is widely used in gas separation of IGCC fuel gas by the hydrate method. In this work, polystyrene nanoparticles grafted by –SO3– groups (−SO3–@PSNS) and grafted by –SO3– groups and Ag particles (Ag&–SO3–@PSNS) are used together with TBAB, respectively, to promote the formation of hydrate. The gas separation effect and growth morphology are studied. The experimental results demonstrate that the incorporation of nanopolymer can significantly enhance the separation efficiency (SFr) of a mixture of H2 and CO2. Notably, compared to the reaction solution without nanopolymer, 2 mmol/L –SO3–@PSNS exhibits the most pronounced effect on gas separation, resulting in an impressive gas consumption of 0.755 ± 0.323 mmol/L and a remarkable increase in the separation factor (SF) by 106%. After loading silver nanoparticles, the promoting effect of Ag&–SO3–@PSNS is further strengthened. Under Ag&–SO3–@PSNS-20%, the gas consumption reaches the maximum of 0.775 ± 0.003. Under Ag&–SO3–@PSNS-30%, the SF rises from 32.79 ± 6.27 to 37.92 ± 7.19, indicating an impressive increment of 15.80%. The visualized droplet experiment shows that Ag&–SO3–@PSNS significantly promotes the nucleation of hydrate and the growth rate of hydrate.
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Journal of Energy Chemistry
·
2025
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IF 14.9
Chaoran Yang,Shuyu Liang,Cong Zhang,Tianyu Zhang,Wenfu Xie,Min Li,Qiang Wang
Copper (Cu)-based catalysts have demonstrated promising selectivity and activity in electroreducing CO 2 to multi-carbon (C 2+ ) products. Among them, oxide-derived Cu catalysts exhibit high selectivity for C 2+ products in the CO 2 electroreduction reaction (CO 2 RR). Cu chalcogenide-derived catalysts offer a promising approach to tune the electronic structure of Cu sites via surface reconstruction, thereby affecting the product distribution. However, the effect of in-situ anion dissolution, especially Se ions, on the electronic structure of Cu selenides at negative potentials remains overlooked, despite its potential to significantly affect catalytic activity. In this study, we developed a series of Cu selenide catalysts with varying Cu/Se ratios to optimize electronic structures and enhance CO 2 RR performance. Among them, Cu 1.8 Se, featuring Cu vacancies, exhibited the highest activity for C 2+ products formation and the highest C 2+ /C 1 products ratio, nearly 2–3 times greater than the others. This catalyst also demonstrated good stability over 38 h of electrolysis under −450 mA cm −2 , with a maximum C 2+ products Faradaic efficiency (FE) of up to 70 %. In-situ surface reconstruction analysis revealed Se loss and Cu + /Cu 2+ reduction of the initial Cu 1.8 Se catalyst, forming Cu/Cu x Se structures with Cu vacancies, identified as the real active sites. Density functional theory (DFT) calculations and in-situ infrared absorption spectroscopy confirmed that Cu vacancies play a critical role in stabilizing *CHOCO intermediates for C–C coupling while suppressing hydrogen evolution reaction and C 1 products formation. These findings highlight Cu vacancy engineering as an effective strategy for enhancing C 2+ selectivity in CO 2 RR.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2025
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IF 5.4
Yulan Xu,Minxian Wu,Xianxian Zhang,Wenchang Wang,Naotoshi Mitsuzaki,Zhidong Chen
Electrodeposition is a simple and rapid method for the preparation of thin-film materials, allowing catalytic materials to be directly deposited onto substrates, thereby eliminating the need for binders. Compared with bulk materials, two-dimensional thin films possess a higher specific surface area. The incorporation of Ga in Sn-based alloy materials can effectively expose active sites, thereby enhancing the catalytic performance for CO 2 electroreduction. Doping with rare-earth elements such as cerium can induce the formation of oxygen vacancies and defect sites, or modulate the electronic structure of the catalyst surface. These modifications enable independent regulation of the adsorption energy of various intermediates, effectively lowering reaction energy barriers and improving catalytic efficiency. In this work, Ga-Sn-Ce electrodes were synthesized via electrodeposition in a deep eutectic solvent composed of choline chloride and urea, and subsequently applied to CO 2 reduction. The GaSnCe0.6 electrode exhibited excellent selectivity toward formic acid at −0.99 V vs. the reversible hydrogen electrode, achieving a Faradaic efficiency of 92 %. Compared with previously reported Ga-Sn alloys, the introduction of Ce resulted in a positive shift of 250–270 mV in the optimal reduction potential for formic acid production from CO 2 .
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Carbon Capture Science & Technology
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2025
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IF 10.5
Hui Zhou,Yaozu Wang,Yuqi Niu,Yunrong Zhao,Bocheng Yu,Jinyang Xu,Yongqing Xu,Shijie Yu,Xuan Bie,Qinghai Li,Yanguo Zhang,Jingyuan Ma,Shuzhuang Sun,Fei Song
The incorporation of nitrate molten salts has been demonstrated as an effective strategy to enhance the CO 2 uptake of MgO for intermediate-temperature (200–400°C) CO 2 capture. However, the slow carbonation kinetics in flue gas capture, coupled with poor stability, hinder its industrial application. In this study, the addition of Na 2 CO 3 was found to significantly improve the sorption kinetics of MgO in a 15% CO 2 atmosphere, achieving a CO 2 capacity of 19.9 mmol/g at 275°C with a 15 mol% total promoter loading (Na 2 CO 3 /NaNO 3 = 1:4). Mechanistic analysis revealed that Na 2 CO 3 promotes the formation of Na 2 Mg(CO 3 ) 2 , which acts as an effective nucleation site for MgCO 3 formation, accelerating the carbonation rate by a factor of eight. The Hard X-ray photoelectron spectroscopy (HAXPES) revealed that an increased Na/Mg ratio caused subsurface migration and aggregation of molten salts, leading to a permanent rise in local salt concentrations, which negatively affected CO 2 capture performance. These findings offer valuable insights into the structural degradation mechanisms and provide guidance for enhancing the stability of nitrate-enhanced MgO, thereby improving its potential for intermediate-temperature CO 2 capture.
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ADVANCED FUNCTIONAL MATERIALS
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2025
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IF 19
Mingxiu Lv,Hao-Nan Li,Jia-Hui Xin,Guang-Chang Xu,Shuhui Ma,Chuang-Wei Gu,Zhanbo Li,Zherui Chen,Chao Zhang,Yajun Deng,Xiao-Jun Huang,Zhi-Kang Xu
Ionic liquids (ILs) featuring excellent selective solubility for CO 2 have led to versatile development and applications of gas separation membranes for CO 2 capture. Over the past decade, a myriad of ILs-based membranes have been exploited; however, they normally suffer from a formidable conflict between CO 2 permeance and stability as imposed by their mutually exclusive design requirements. Herein, a photothermal-steered confined gelation and locking engineering (CGLE) is proposed to fabricate ultrathin dual-confined ionogel membranes (DCIMs) that empower ultrapermeable and durable CO 2 separation. In the CGLE, coupling CNTs-enabled photothermally confined reactor with ILs-regulated gelation behavior, ionogel precursors consisting of poly(ethylene glycol) diacrylate and 1-butyl-3-methylimidazolium tetrafluoroborate experience in situ confined polymerization and gelation within CNTs-stacked skeleton, thus making free ILs dually locked via dual confinement of CNTs skeleton and gel network. These DCIMs have a greatly decreased thickness to 1–3 µm by ≈100 folds over counterparts, yet exhibiting an enhanced pressure resistance and long-term stability. Moreover, DCIMs give an ultrahigh CO 2 permeance of 113 GPU, a rewarding CO 2 /N 2 and CO 2 /CH 4 selectivity of 68 and 88, respectively, transcending most ILs-based membranes. These findings represent a paradigm shift in developing advanced ionogel membranes beyond gas separation.
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CHINESE JOURNAL OF CATALYSIS
·
2025
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IF 17.7
Yang Chen,Diwen Zhou,Yongli Chang,Hongqiao Lin,Yunzhao Xu,Yong Zhang,Ding Yuan,Lizhi Wu,Yu Tang,Chengyi Dai,Xingang Li,Qinhong Wei,Li Tan
CO 2 hydrogenation to CH 3 OH is of great significance for achieving carbon neutrality. Here, we show a urea-assisted grinding strategy for synthesizing Cu-Zn-Ce ternary catalysts (CZC-G) with optimized interfacial synergy, achieving superior performance in CO 2 hydrogenation to methanol. The CZC-G catalyst demonstrated exceptional methanol selectivity (96.8%) and a space-time yield of 73.6 g MeOH ·kg cat –1 ·h –1 under optimized conditions. Long-term stability tests confirmed no obvious deactivation over 100 h of continuous operation. Structural and mechanistic analyses revealed that the urea-assisted grinding method promotes the formation of Cu/Zn-O v -Ce ternary interfaces and inhibits the reduction of ZnO, enabling synergistic interactions for efficient CO 2 activation and selective stabilization of formate intermediates (HCOO*), which are critical for methanol synthesis. In-situ diffuse reflectance infrared Fourier transform spectra and X-ray absorption spectroscopy studies elucidated the reaction pathway dominated by the formate mechanism, while suppressing the reverse water-gas shift reaction. This work underscores the critical role of synthetic methodologies in engineering interfacial structures, offering a strategy for designing high-performance catalysts for sustainable CO 2 resource utilization.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-10
·
IF 15.7
Li Hao-Nan,Sun Ze-Yu,Yu Zhen-Jie,Man Kexin,Zhang Chao,Xu Zhi-Kang
Mixed matrix membranes (MMMs) capable of breaking the permeability-selectivity trade-off suffer from the inefficient and disconnected bulky transport channels as well as inferior interfacial compatibility between nanomaterials and polymers. Herein, we propose an original photothermal-triggered in-situ gelation approach to elaborate an original class of MMMs, termed nanofiber-interwoven gel membranes (NIGMs) that feature tunable 3D-interconnected ultrafast transport channels and highly-selective CO 2 -philic gel for boosting CO 2 separation performance. The key design of NIGMs lies in leveraging dual functions of CNT-interwoven skeleton: (1) serving as a photothermal confined reactor that rapidly triggers in-situ gelation of highly-selective CO 2 -philic gel without phase separation-induced interfacial defects to construct defect-free and thickness-controllable NIGMs; (2) functioning as a 3D-interconnected continuous skeleton for providing ultrafast CO 2 transport channels. By orchestrating the distribution and configuration of interwoven nanofibers, the NIGMs possess a boosted CO 2 permeance of 211.0 GPU increased by 1558% over polymeric gel counterparts and an ultrahigh CO 2 /N 2 and CO 2 /CH 4 selectivity of up to 151 and 47 respectively. Our work offers a paradigm shift in developing advanced MMMs beyond gas separation.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-13
·
IF 15.7
Gong Shanhe,Zhai Yanjie,Jin Chengkai,Xu Han,Xia Qing,Li Weisong,Ying Yiran,Wu Jie,She Xiaojie,Wang Zhaolong,Lv Xiaomeng,Wu Chundu,Chan Kangcheung,Zhao Xunhua,Zhang Xiao,Lau Shu Ping
Electrochemical carbon dioxide reduction reaction (CO 2 RR) under strongly acidic conditions enables high CO 2 utilization. However, especially in proton exchange membrane (PEM) electrode assembly reactors, achieving selective CO 2 RR in such environments remains challenging due to uncontrolled interfacial water diffusion at high current densities. Here, we develop a nickel-based heterogeneous molecular electrocatalyst (NiPc-NH 2 /CNT-SHP) featuring amino (-NH 2 ) functional groups and grafted long-chain hydrophobic molecules. Under acidic conditions, -NH 2 is in situ protonated to form amino cations (-NH 3 ⁺). The positively charged -NH 3 ⁺ groups and hydrophobic molecules effectively disrupt the protonated water (H 3 O + )-rich network, inhibiting the invasion of H 3 O + and thereby suppressing the hydrogen evolution reaction, while enhancing selectivity for acidic CO 2 RR. The catalyst achieves nearly 100% Faradaic efficiency for CO at current densities from 50 to 400 mA cm −2 , with approximately 76% CO 2 utilization efficiency in a flow cell, and sustains over 80% selectivity for more than 200 h in a self-designed PEM–porous solid electrolyte reactor. These findings highlight interfacial water management as a key design principle for efficient acidic CO 2 electroreduction.
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