ACS Catalysis
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2025
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IF 13.1
Qiyou Wang,Yusen Xiao,Feng Li,Yao Tan,Yuxiang Liu,Franz Gröbmeyer,Kang Liu,Junwei Fu,Hongmei Li,Cheng-Wei Kao,Ting-Shan Chan,Rui-kai Miao,Liyuan Chai,Emiliano Cortés,Min Liu
In acidic CO2 electroreduction reaction (CO2RR), excessive H* adsorption from high proton concentrations suppresses *CO coverage on Cu-based catalysts, limiting multicarbon (C2+) product formation. Here, we introduce a K+ insertion strategy via an interlayer electric field (IEF) between the layers of Cu nanosheets (K+-Cu NS) to strengthen *CO adsorption and boost C2+ selectivity. Finite element method (FEM) simulations verified the role of the IEF in enriching K+ ions, meanwhile density functional theory (DFT) calculations demonstrated these enriched K+ ions facilitate stronger *CO adsorption. Ar+ ion-etching-assisted X-ray photoelectron spectroscopy (XPS) and operando Raman spectroscopy confirmed the structured K+ stuffing. Operando attenuated total reflection infrared spectroscopy (ATR-IR) demonstrated the enhanced *CO adsorption on K+-Cu NS. As a result, the K+-Cu NS catalyst achieved an ultrahigh cathodic energy efficiency of 42.5% and a remarkable Faradaic efficiency of 80.3% for C2+ products in a flow cell. This work highlights a novel cation regulation strategy for advancing the acidic CO2RR efficiency.
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ACS Catalysis
·
2025
·
IF 13.1
Teng Xu,Guilin Yin,Fengyu Wang,Fan Yang,Junli Xu,Jinyu Ye,Danfeng Wu,Xiaoxu Duan,Weng Fai Ip,Sen Lin,Haifeng Xiong
Integrated CO2 capture and electrochemical utilization (ICCU) is promising for decarbonization by bypassing energy-intensive desorption/compression steps compared to conventional CO2 capture and utilization (CCU) systems. However, the critical barrier in ICCU is the mass transfer limitations of carbon-containing species from amine solutions to electrode surfaces, leading to a low CO2 conversion and a high hydrogen evolution reaction (HER). To address this issue, we introduce an interfacial engineering strategy to create a microenvironment using quaternary ammonium cationic surfactants for enhanced CO2 conversion. In the cetyltrimethylammonium bromide (CTAB)-modified monoethanolamine (MEA) system, a Ag nanoparticle achieved 63.4% CO Faradaic efficiency at −0.82 V vs RHE, representing a 4.7-fold improvement over unmodified system. Chain-length optimization revealed that short-chain surfactants lacked sufficient hydrophobicity, while long-chain variants increased the mass transfer resistance, positioning CTAB (C16) as the optimal candidate. The strategy demonstrates amine versatility and 50 h of recyclability without catalyst/amine degradation. In situ spectra and density functional theory calculation elucidated that CTAB has dual roles, i.e., CTAB cation (CTA+) adsorption repels the aggregation of protonated amine (MEAH+) on the electrode surface and the hydrophobic alkyl chains enrich the carbon-containing species. This work provides a mechanistic framework for designing efficient and stable ICCU systems through creating a microenvironment.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
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IF 9
Xueru Zhao,Jinlong Wu,Jiaxin Bai,Ting Zhang,Zhenli Lv,Maoxu Wang,Min Zhu,Jing Li,Feng Li
Cuprous oxide (Cu 2 O) is a promising material for photoelectrocatalytic CO 2 reduction (PEC-CO 2 RR); however, its widespread application is hindered by issues such as photocorrosion, structural instability, and low selectivity toward desirable products. In this work, a Cu 2 O-BiOBr nanohybrid catalyst with excellent visible light responsiveness are successfully developed using energy band structure matching and morphology modulation strategies. This heterostructure exhibits a three-dimensional bridge-like architecture composed of interwoven one-dimensional nanorods and two-dimensional nanosheets. Cu 2 O acts as a surface electron-rich active center, while BiOBr functions as both a co-catalyst and photogenerated electron storage, enabling efficient photoelectrocatalytic conversion of CO 2 under visible light irradiation. That is, the optimized Cu 2 O-BiOBr-2 catalyst achieves a C 2+ Faraday efficiency (FE) of 51% at −0.6 V vs. RHE, which is 2.55 times exceeding the pure Cu 2 O catalysts, The findings obtained from in-situ spectroscopic characterization reveal that the efficient transport channel of the constructed heterojunction enhances charge transfer efficiency at the catalyst interface and boosts redox capacity, improving both efficiency and stability of Cu 2 O in PEC-CO 2 RR. This work provides new insights for constructing novel heterojunctions.
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ENERGY & FUELS
·
2025
·
IF 5.3
Guang Miao,Pengxian Ye,Junyang Wang,Jiawu Huang,Jing Xiao,Chunshan Song
The development of cost-effective, high-performance sorbents for CO2 capture in hydrogen purification remains a critical challenge, particularly under industrial conditions of ultralow CO2 concentrations and ambient temperatures. This study systematically investigates polyethylenimine (PEI)-impregnated SiO2 and SBA-15 sorbents, with a focus on enhancing CO2 uptake and kinetics through polyethylene glycol (PEG) incorporation. Although PEI-SBA-15 sorbents showed higher static and dynamic CO2 uptakes compared to PEI-SiO2 sorbents, its diffusion barrier lowers the adsorption rate in the flow system. The poly(ethylene glycol) (PEG) polymers were introduced to PEI-SiO2 to improve the mass transfer of CO2 in PEI clusters. The low PEI loading was found to be beneficial to CO2 adsorption on SiO2, resulting in superior CO2 uptakes and a lower diffusion barrier than PEI-SBA-15 sorbents. The characterization was conducted to uncover physical and chemical properties. The breakthrough experiments of PEI-30-SiO2 with PEG derivates confirmed that the O in the skeleton of PEG played an important role in the interaction between PEI and PEG rather than terminal OH groups. This work also demonstrated the CO2 desorption and stability of PEG-modified PEI-SiO2 sorbents in H2.
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Materials Chemistry Frontiers
·
2025
·
IF 6.4
Yapeng Dong,Yuning Liang,Bo Gao,Qun Xu
Exploring advanced technology to obtain quantum materials presenting novel and unexpected electronic states upon proper manipulation is an important research endeavor. Usually, plastic deformation can lead to some amount of disruption that can result in new physical phenomena and fascinating structures. However, how to realize efficient plasticization and manipulation to obtain irreversible variation in such materials, especially those presenting quantum material behavior, is a great challenge. Herein, we show that upon plastic deformation induced by supercritical CO2 (SC CO2) on SrZrO3, typically at a pressure of 16 MPa, SrZrO3 experiences a transition from a bulk material to a two-dimensional (2D) structure. More importantly, it can be observed that the octahedral rotation of ZrO6 is suppressed. Furthermore, plastic deformation frequently induces magnetism in SrZrO3. Via polarization characterization, SrZrO3 displays multiferroic characteristics, exhibiting a considerable enhancement in the saturation magnetisation strength and polarization strength. At room temperature, SrZrO3 exhibits a saturated magnetisation of 0.1280 emu g−1, accompanied by a polarization of 0.27 μC cm−2. Therefore, this work demonstrates that plastically deformed SrTiO3 induced by SC CO2 can successfully transition into a quantum multiferroic material. These results establish a new method toward plastic deformation for the manipulation of the electronic properties of quantum materials.
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ACS Catalysis
·
2024
·
IF 11.3
Yueqi Feng,Jiaomei Xiao,Yiyi Qiu,Jianlin Huang
Precise control and understanding of surface changes in indium (In)-based catalysts during the electrocatalytic CO2 reduction reaction (CO2RR) process are challenging. This study presents a series of surface-reconstructed In2O3–Bi electrocatalysts, created by doping mesoporous In2O3 nanocubes with bismuth (Bi). This doping introduces abundant bimetallic In–Bi sites at the crystal–amorphous interfaces, enhancing the CO2-to-formate conversion selectivity. Bi atoms accelerate the surface reconstruction of In2O3, reduce the charge density around In atoms, and promote partial amorphization. In situ X-ray diffraction (XRD) and Fourier-transform infrared spectroscopy (FT-IR) measurements and density functional theory (DFT) calculations show that the bimetallic In–Bi sites lower the energy barrier for the HCOOH* intermediate, enhance H2O dissociation, and inhibit the hydrogen evolution reaction (HER). The surface-reconstructed In1.8Bi0.2O3 electrocatalyst demonstrates a Faradaic efficiency (FE) of 92.6% and a partial current density of −28.5 mA·cm–2 and operates stably for 110 h in a H-type cell. In a flow cell, it achieves an FE of formate (FEformate) of 97.6% at −1.4 VRHE and maintains above 94% FEformate over a potential window of 800 mV (from −1.0 to −1.8 V vs RHE). This study offers an effective approach for designing high-performance electrocatalysts for the CO2RR based on surface reconstruction.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2024
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IF 3.8
Xiaojiang Li,Xingqiao Zhang,Chengwei Zuo,Han Zhang,Zhenfu Jia
Cleaner recovery of petroleum hydrocarbons is a key process for waste oil and gas resources, especially oily waste solid. However, the direct recovery of petroleum hydrocarbons is difficult with deep eutectic solvents (DES) without other additives (such as water). In this work, ionic liquid-based DESs (ILs-DESs) with a controllable polarity were prepared for the sustainable recovery of petroleum hydrocarbons. Here, CO2-responsive ionic liquids were prepared by the neutralization reaction of 1,8-diazabicyclo[5.4.0]undec-7-ene and iminazole (Im), pyrazol (Py), or triazole (Tri). Then, the ILs-DESs were separately prepared by using ionic liquids as proton acceptors and straight-chain alcohols (carbon number = 4, 6, 8, 10, and 12) as proton donors. The polarity transformation of the ILs-DESs was regulated only by the introduction and removal of CO2, which was caused by the reversible transformation from ILs-DESs with a lower polarity to alkyl carbonate and carbamate with higher polarity upon CO2. Because of the polarity changes, the simulated oil (such as n-dodecane or diesel oil) was mixed with ILs-DESs, and the samples were directly separated by introducing CO2. Finally, a sustainable process for treating oil sands and oily sludge by using ILs-DESs was developed, where the ILs-DESs were also reused more than twice. This implies that a sustainable approach for petroleum hydrocarbon recovery was realized by using DESs.
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ADVANCED FUNCTIONAL MATERIALS
·
2024
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IF 18.5
Sheng Li,Xin Yu,Liming Liu,Liqin Zhou,Zhaowei Jia,Jianmin Chen,Zhongxing Zhao,Zhenxia Zhao
Synchronous boosting adsorption and desorption efficiency is a great challenge for CO 2 adsorption capture, especially for metal–organic frameworks (MOFs) having high adsorption uptakes. Herein, a novel “self-supporting foam” strategy is proposed to fabricate a thermally conductive MOFs@boron nitride nanosheets (BNNS) composite foam (MOFs@BNNS-PEI) via polyethyleneimine (PEI) cross-linkage. The “rebar” BNNS and the “aggregate” MOFs are packed against each other to form a self-supporting structure, effectively reducing the reliance on polymers to maintain high MOFs loading. Furthermore, this approach enables the successful fabrication of three different types of typical MOFs, including HKUST-1, MIL-100(Fe), and ZIF-8. This unique design maintains a high specific surface area (SSA) of the MOFs foam and generates nitrogen-rich microporosity contributing to CO 2 adsorption. Additionally, PEI serves as a thermal bridge to reduce the interfacial thermal resistance between BNNS and MOFs, accelerating the thermal desorption of CO 2 within the MOFs foam. Benefiting from these advantages, the MOFs@BNNS-PEI exhibits a higher CO 2 adsorption capacity (1.35–1.42 times that of pure MOFs) and a significant increase in the desorption rate for CO 2 (5.0–5.7 times that of pure MOFs). Thus, the thermally conductive MOFs foam can be a viable option for efficient CO 2 capture in practical applications.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Siyao Wang,Jingfa Zhang,Yongchao Sun,Fangxu Fan,Qizheng Zhao,Gaohong He,Canghai Ma
Thermally rearranged (TR) polymers are increasingly pivotal in gas separation membranes, with a pressing need for advancements in mechanical strength and separation performance. In this work, a novel variety of TR polymers were synthesized by polymerizing an amine-functionalized triptycene structure with thermally rearrangeable ortho -hydroxy groups. The TR membranes demonstrate enhanced gas permeability in H 2 /CH 4 and CO 2 /CH 4 tests and increased polymer chain spacing. Additionally, incorporating triptycene enhanced the mechanical properties of TR polymers, primarily attributed to the π-π stacking interactions of the triptycene units. Notably, the 6FDA-BAP:DAT (2:1) membrane thermally rearranged at 400 °C exhibited a H 2 permeability of 225.3 Barrer and a H 2 /CH 4 selectivity of 146.3, representing increases of 320 % and 154 %, respectively, compared to the precursor, and surpassing the H 2 /CH 4 upper bound. This work presents a robust design strategy for preparing mechanically durable TR membranes with enhanced gas separation performance.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-15
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IF 15.7
Cai Zhongjie,Liu Hongwei,Dai Jiajun,Li Bao,Yang Liming,Wang Jingyu,Zhu Huaiyong
Overall artificial photosynthesis, as a promising approach for sunlight-driven CO 2 recycling, requires photocatalysts with efficient light adsorption and separate active sites for coupling with H 2 O oxidation. Here we show a In-based metal–organic framework (MOF) heterostructure, i.e., In-porphyrin (In-TCPP) nanosheets enveloping an In-NH 2 -MIL-68 (M68N) core, via a facile one-pot synthesis that utilises competitive nucleation and growth of two organic linkers with In nodes. The coherent interfaces of the core@shell MOFs assure the structural stability of heterostructure, which will function as heterojunctions to facilitate the efficient transfer of photogenerated charge for overall photosynthesis. The In-TCPP shell in MOFs heterostructure improves CO 2 adsorption capabilities and visible light absorption to enhance the photocatalytic CO 2 reduction. Simultaneously, In-O sites in M68N core efficiently catalyze H 2 O oxidation, achieving high yields of HCOOH (397.5 μmol g −1 h −1 ) and H 2 O 2 (321.2 μmol g −1 h −1 ) under focused sunlight irradiation. The superior performance of this heterostructure in overall photosynthesis, coupled with its straightforward synthesis, shows great potential for mitigating carbon emissions and producing valuable chemicals using solar energy.
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Science Bulletin
·
2025
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IF 21.1
Wanguo Gao,Zhe Lu,Yecheng Leng,Chengyang Wu,Yingfang Yao,Xi Zhu,Junchuan Sun,Xiwen Yu,Cheng Wang,Congping Wu,Wenlei Wu,Bing Wang,Lu Wang,Zhigang Zou
Cu-based catalysts attract considerable attention because of their exceptional CO 2 photo-/electro-/thermo-reduction capacities, where Cu(I) is generally treated as the active species. However, a significant problem hindering the large-scale applications of Cu-based catalysts is the inactivation of Cu(I) via irreversible redox to Cu(II)/Cu(0). This study proposes a Cu(I) valence pinning method based on hydroxyapatite (HAP). Experimental and theoretical studies demonstrate that the phonon resonance among the Cu(I) ions, their adjacent heteroatoms, and the intermediates adsorbed at the Cu(I) sites yields Cu(I) valence electrons in their lowest energy states. Thus, Cu(I) is stabilized, stable, and efficient photothermal CO 2 hydrogenation is promoted. However, because of the change of Cu(I) coordination environment during the CO 2 hydrogenation reaction, Cu(I) ions migrate into the bulk phase, leading to activity attenuation. Nevertheless, Cu(I) ions can be pulled out to the surface of HAP under the oxidative humid air condition, and the catalytic activity can be easily recovered. Thus, we propose a simple cyclic reaction/regeneration process. This enables the Ca 5 (FeCuCe) 5 -HAP catalyst to achieve the CO yield of 402.8 mmol g −1 h −1 and a CO 2 conversion rate of 27.7%, which is close to the thermodynamic equilibrium. This catalyst also displays a selectivity of approximately 100% and cycle stability of 156 h at 500 °C under a pressure of 1 atmospheric. Our study provides a viable method for the scale applications of Cu(I) based catalysts in the “negative carbon” industries.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
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IF 21.1
Shuzhuang Sun,Bocheng Yu,Weiwen Meng,Yongqing Xu,Yanmei Shen,Zhehao Sun,Zongyou Yin,Hongman Sun,Hui Zhou,Hengshan Qiu
Understanding the dynamic phase change under operational conditions is crucial for the development of high-performance catalysts. Ni-based alloys have long been elucidated as active and selectivity-tunable phases in CO 2 hydrogenation, while their gas-dependent surface reconstruction and correlation with dynamic activities, particularly under gas-swing catalytic conditions, remain poorly understood. Herein, we demonstrate that Zn can segregate from the NiZn alloy in a CO 2 atmosphere enabling formation of well-dispersed surface Ni atoms that can gradually homogenize back into the alloy under H 2 . Consequently, formation of highly stable intermediates, bridged and multi-centered carbonyls, can be effectively avoided due to the absence of closely-packed Ni sites. Instead, the linear carbonyls on Ni undergo desorption rather than further hydrogenation due to their relatively low binding energy, rendering a high CO selectivity. This insight of gas-dependent evolution of sites will enable the rational design of alloy catalysts for multi gas swing catalytic applications.
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