ACS Nano
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2026
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IF 16
Yong Su,Junli Xu,Jia Zhao,Congcong Du,Qiunan Liu,Jiwei Li,Sixu Liu,Zhun Zhang,Yang Luo,Lin Geng,Jingzhao Chen,Kelvin H. L. Zhang,Yongfu Tang,Liqiang Zhang,Qiao Huang,Kazu Suenaga,Feiteng Wang,Jun Cheng,Sen Lin,Wei Tan,Lin Dong,Fudong Liu,Jianyu Huang,Haifeng Xiong
Metal single-atom catalysts (SACs) offer exceptional atomic efficiency and remarkable properties, making them highly valuable for energy and environmental applications. However, existing SAC preparation methods face challenges, such as the need for high temperatures or limitations in metal loading. In this study, we present a room-temperature synthesis strategy for stable SACs with high metal loadings (>10 wt %), achieved through electrochemical redox reactions within lithium-ion batteries. The reaction mechanism was thoroughly elucidated, revealing that bulk metallic compounds (denoted as MaXb, where M represents a metal and X is F, S, or O) disintegrate from the millimeter scale down to single atoms at room temperature. This process is driven by lithiation–delithiation-induced grain refinement and the dissolution of metals, which are subsequently captured by the substrate. The resulting single-atom catalyst (e.g., Cu SAC) demonstrates outstanding reactivity for electrocatalytic CO2 reduction, showcasing excellent electrochemical stability and superior performance. This room-temperature redox method is versatile and compatible with a wide range of metals and supports, highlighting its potential for broad applications in sustainable catalytic technologies.
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Carbon Neutrality
·
2026
·Vol. 5
·期 1
·4
·
IF 12.5
Wang Shaona,Yang Yang,Xu Wenqing,Bai Zhuoshu,Su Fabing,Wang Yixi,Bai Dingrong,Zhu Tingyu
As an integrated CO 2 capture and utilization (ICCU) process, direct electrochemical reduction of amine captured-CO 2 reduction reaction (cCO 2 RR) has enormous advantages in energy efficiency and operating cost. The low product selectivity is an urgent issue. Here, we found that the hydroxyl (-OH) on CeO 2 can significantly enhance CO selectivity. After hydroxyl modification, the CO faraday efficiency (FE CO ) was surprisingly increased by 188% (relative increase rate). The correlation coefficient between -OH quantity and FE CO is as high as 0.98. Further study indicated that the presence of -OH can lead to a more compact electrochemical double layer (EDL) and charge transfer resistance by proton transfer. The -OH can also enhance CO 2 adsorption and stabilize the intermediate species (*COOH). DFT results further demonstrate that the rate-determining step was proton transfer from the surface -OH to MEACOO − , -OH modification can reduce the energy barrier to as low as 0.39 eV. This work provides additional insights into improving selectivity in amine-based cCO 2 RR, advancing the development of ICCU technology.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2026
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IF 9
You-yun Gong,Xuejing Zhang,Jin-ping Cheng
Metal–organic frameworks (MOFs) offer tunable porosity and chemistry for advancing CO 2 capture. In this work, a ‘thermal-annealing–amine vapor deposition' strategy is proposed to synergistically engineer structural defects and uniformly distributed amine functionalities in UiO-66. Controlled annealing generates defect-rich UiO-66 (UiO-66-D) with exposed Zr 6 clusters, while subsequent hydrazine vapor deposition anchors amine groups directly at defective Zr nodes. The optimized material, N 2 H 4 @UiO-66-D, exhibits a markedly increased surface area (1449.36 m 2 /g) and achieves a CO 2 adsorption capacity of 2.60 mmol/g (at 298 K, 1 bar and pure CO 2 )—significantly higher than pristine UiO-66 (1.44 mmol/g at 298 K, 1 bar and pure CO 2 ). Enhanced CO 2 /N 2 separation performance is observed under simulated flue-gas conditions (at 1 bar, 298 K and 15 % CO 2 /85 % N 2 ), with IAST selectivity in the range of 111–33. Cyclic adsorption–desorption tests show no obvious decay in CO 2 uptake after ten cycles. Molecular dynamics (MD) simulations reveal that hydrazine modification increases free volume near defect sites, enhancing local CO 2 density. Density functional theory (DFT) calculations show that CO 2 preferentially adopts a bidentate surface adsorption (‘face-on') configuration at hydrazine-modified Zr defects, with an adsorption energy of −0.33 eV, confirming strong CO 2 activation and favorable binding. This work establishes a mechanistic framework for coupling defect engineering with vapor-phase amine functionalization, providing transferable design principles for the development of MOF-based CO 2 adsorbents.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 13.2
Siyuan Huang,Xia Wang,Jia Liu,Bilyu Hong,Kai Yuan,Youzhu Yuan
Catalytic conversion of CO 2 to light aromatics (including benzene, toluene, and xylene, collectively known as BTX) and olefins is an eco-friendly approach for reducing waste gas emissions, but it remains a significant challenge. Traditional methods that modify the surface acid sites of zeolites to increase BTX selectivity often produce undesired byproducts and involve complex preparation processes. Here, we report a strategy to enhance BTX formation by altering the reaction intermediates using a tandem catalyst composed of metal oxides and dual-zeolite (GaZrO x /SAPO-34/ZSM-5, labelled as GZO/S34/Z5). The inclusion of S34 zeolite facilitates the partial transformation of CO 2 hydrogenation intermediates produced by GZO into light olefins, thereby promoting the aromatic formation in Z5. This results in a 72.6 % selectivity for total aromatics in hydrocarbons, with BTX accounting for a significantly higher selectivity compared to GZO/Z5, representing a 3.4-fold increase from 7.1 % to 24 %. Additionally, by regulating the acid density of Z5, the tandem catalyst with dual-zeolite can directly convert CO 2 and H 2 to 53.5 % aromatics and 25.5 % olefins, with a BTX selectivity of 13.8 % in hydrocarbons. This tandem catalyst design, through adjusting the reaction intermediates, offers an efficient method to inhibit the formation of light paraffin byproducts and enhance BTX selectivity in CO 2 conversion.
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JOURNAL OF MEMBRANE SCIENCE
·
2026
·
IF 8.8
Shucheng Tian,He Tao,Zhifang He,Tingting Chang,Bin Li,Jianye Li,Xueqing Li,Lu Wang,Zibo Yang,Zhihua Qiao
Ti 3 C 2 T x is a two-dimensional sheet-like material with abundant and tunable surface functional groups, showing excellent gas adsorption and transport ability in CO 2 separation. However, it suffers from several intrinsic limitations, including susceptibility to oxidation, restacking, and humidity sensitivity, which prevent it from being used alone as a membrane material for complex application scenarios. In this work, meltable ZIF-62 was selected as the continuous phase and Ti 3 C 2 T x as the dispersed phase. Thermal treatment was used to promote the softening and flow of ZIF-62, enabling the embedding and immobilization of Ti 3 C 2 T x . Finally, self-supporting Ti 3 C 2 T x /a g ZIF-62 composite glass membranes were obtained, and their gas separation performance was evaluated. The results show that the introduction of Ti 3 C 2 T x effectively improves the CO 2 permeability of the composite membranes while maintaining high separation selectivity. Specifically, the best overall performance was achieved at a doping content of 1 wt%, where the CO 2 permeability increased from 1403 Barrer to 5124 Barrer, and the ideal CO 2 /N 2 and CO 2 /CH 4 selectivities reached 44.9 and 30.7, respectively. The CO 2 /N 2 separation performance of this membrane exceeds the latest upper bound, while its CO 2 /CH 4 separation performance also shows a competitive level. In addition, this membrane maintained relatively stable performance in humid-gas, pressure-variable, and 160 h continuous operation tests.
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ENERGY & FUELS
·
2026
·
IF 6
Jiayou Liao,Junling Lin,Shuangming Wang,Zhichao Zhai,Xianjie Meng,Yangyang Wang,Yong Wang,Chengyun Gao,Fanhui Meng,Jinping Li
Mixed matrix carbon molecular sieve membranes are gas separation membranes that combine the synergistic effects of carbon molecular sieves and inorganic components. The DD3R molecular sieve exhibits significant molecular size sieving effects and demonstrates high adsorption selectivity toward CO2. Against the backdrop of the current push for carbon neutrality, highly efficient CO2 separation materials are of great significance to the development of carbon capture and storage (CCS) technology. This is particularly true in natural gas purification and industrial exhaust gas treatment, where higher demands are placed on the efficient separation of CO2 and CH4. Based on this, this study used the DD3R molecular sieve as the functional filler, used 6FDA-DAM polyimide as the precursor, and obtained the hybrid matrix carbon membrane through a high-temperature carbonization process. The microstructure and physicochemical characteristics of the carbon membranes were systematically characterized using scanning electron microscopy and other techniques, and the effect of DD3R loading on their gas separation performance was investigated. The results indicate that as the doping concentration of DD3R molecular sieves increases, both the CO2 permeability and CO2/CH4 separation selectivity of the mixed matrix carbon molecular sieve membranes exhibit a trend of initially increasing and then decreasing. Furthermore, when the DD3R doping mass fraction reached 0.3 wt %, the prepared carbon membrane exhibited optimal performance, achieving a CO2 permeability coefficient of 29,679 Barrer and a CO2/CH4 selectivity of 33.1, surpassing the Robeson upper limit reported in 2019. The results indicate that, owing to the unique pore structure of the DD3R molecular sieve and its synergistic interaction with the carbon matrix, the carbon membrane effectively overcomes the trade-off between permeability and selectivity, demonstrating significant potential for industrial applications and holding broad prospects in the field of carbon capture.
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
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2026
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IF 6.7
Xianglong Li,Zhicong He,Haoxian Huang,Yachuan Yuan,Yanbin Feng,Wei Peng,Song Xue
2,4-Dihydroxybenzoic acid is an important intermediate in agricultural and food chemistry. Salicylic acid decarboxylase catalyzes the carboxylation of resorcinol with CO2 to yield 2,4-dihydroxybenzoic acid. However, this process suffers from poor regioselectivity and low carboxylation activity. Here, we propose that the unique microenvironment created by the enzyme’s substrate-binding pocket, referred to here as the enzyme field, induces charge redistribution in resorcinol, thus altering the enzymatic regioselectivity. Charge distributions at carbon atoms were calculated under 14 different enzyme fields, and catalytic assays revealed the correlation between regioselectivity and the electronegativity of the corresponding carbon atom. Furthermore, K23A/Y64T/E291D/Y27A was obtained with 99% C4-carboxylation selectivity from 20%, and a 69-fold increase in kcat/Km. The SAD-catalyzed carboxylation mechanism involving HCO3–-mediated proton transfer was proposed on the basis of QM/MM metadynamics simulations. This work elucidates the repurposing of regioselectivity by enzyme-induced substrate charge distribution and proposes the mechanism of the SAD-catalyzed carboxylation of resorcinol.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2026
·
IF 3.9
Yu-Jiao Li,Qi-Qi Huang,Shi-Chao Qi,Xiao-Qin Liu,Lin-Bing Sun
CO2 adsorption is a key technology for carbon capture. Current applications primarily focus on large-scale industrial CO2 emission sources, while the capture from distributed sources, especially kitchen flue gas, has been ignored. The kitchen flue gas is featured by low CO2 concentrations, high humidity, and high concentrations of volatile organic compounds. Such a complex composition leads to competitive gas adsorption and rapid degradation of the adsorbent performance. Herein, to solve this problem, xP/D-carrier adsorbents are synthesized by coloading polyethylenimine and diethanolamine onto the three SiO2 carriers (fumed silica, hierarchically porous SBA-15, and mesostructured KIT-6). Among them, 0.9P/D-KIT-6 performs the best chemical CO2 adsorption capacity of 2.22 mmol/g at 348 K and 1.0% (vol.) CO2 concentration, showing excellent thermal stability and ultrahigh CO2/N2 selectivity of 1030. Breakthrough tests with simulated kitchen flue gas show that xP/D-carrier adsorbents maintain high CO2 adsorption selectivity under elevated temperatures and complex gas environments.
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Catalysts
·
2026
·Vol. 16
·期 8
·725
·
IF 4.5
Hongtao Xie,Limi Yan,Shijian Lu,Pengcheng Xiang,Dongliang Liu,Lili Wang
The electrocatalytic reduction of CO2into value-added chemicals offers a promising route to mitigate greenhouse gas emissions, yet the uncontrollable structural reconstruction and surface rearrangement of electrocatalysts during operation often lead to severe activity degradation. Herein, we reveal that Bi2O2SO4(BSO) undergoes an irreversible phase transformation into Bi2O2CO3(BCO) nanosheets accompanied by the partial reduction of Bi3+to metallic Bi0under cathodic potentials. A series of BCO/BSO heterojunction catalysts with tunable compositions are synthesized via a mild in situ ion-exchange method. To circumvent the detrimental effects of this dynamic reconstruction, we devise a pre-activation strategy that deliberately completes the structural evolution prior to electrocatalysis. The optimized 20%-BCO/BSO heterojunction achieves a remarkable Faradaic efficiency of 98.4% for formate production in a flow cell at elevated potentials, with >95% FE(HCOOH)over a wide potential window (−0.8 to −1.7 V vs. RHE). In situ infrared spectroscopy elucidates that the reconstructed interface can promote CO2adsorption, stabilize the *OCHO intermediate, and facilitate HCOOH desorption. This work provides experimental evidence of the reconstruction behaviour of bismuth-based catalysts and offers a rational design method for constructing structurally stable heterojunction electrocatalysts.
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JOURNAL OF THE ENERGY INSTITUTE
·
2026
·
IF 6.5
Haifei Wang,Wei Tian,Yunlong Tian,Zhiqiang Han,Chengzhuang Zhang,Kun Liang,Gebrehiwot Gebreslassie,Denggui Wang,Jia Fang
Nitrogen-doped biochars are prepared from corn stalk using different potassium salts (KOH, KHCO 3 , K 2 CO 3 , and potassium citrate) as activators, followed by KCl-assisted modification. Among all samples, PB2 (K 2 CO 3 /KCl co-activated) shows the highest CO 2 uptake of 4.28 mmol/g at 25 °C and 1 bar. This improved performance is attributed to the combined effects of abundant ultramicropores and narrow micropores, particularly pores below 0.6 nm, together with abundant surface functional groups, including graphitic nitrogen and C-N/C-O species. The micropores provide a high density of adsorption sites, which promotes efficient pore filling. Meanwhile, the nitrogen and oxygen functionalities enhance CO 2 affinity by modulating the electronic properties and increasing surface polarity. Cyclic stability is evaluated by thermogravimetric analysis (40 °C, atmospheric pressure). PB2 exhibits an initial CO 2 adsorption capacity of 2.05 mmol/g, which decreases to 1.69 mmol/g after five adsorption-desorption cycles, corresponding to a capacity retention of 82.44%. Although this cyclic performance is lower than those of PB, PB1, and PB3, PB2 combines the highest single-point CO 2 uptake with acceptable cyclic stability. This result indicates a trade-off between adsorption capacity and cycling stability. Overall, the results demonstrate that both pore structure and surface chemistry are critical to CO 2 adsorption performance. Among all samples, PB2 exhibits the most favorable combination of these characteristics.
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Nano Energy
·
2026
·
IF 16.7
Maoxiang Li,Yachao Xu,Shijie Liu,Zihan Ma,Zhaojun Sun,Jianwei Zhang,Ying Wang,Mingyi Zhang
A strained Pd-O-Ti interface with abundant oxygen vacancies forms an electronic potential-well CO-hydrogenation box. • Spatial coupling of CO confinement and hydrogen activation enables exclusive CO 2 -to-CH 4 photoreduction. • This interfacial design provides a general strategy for deep CO 2 hydrogenation products. Solar-driven conversion of CO 2 to methane offers a route to carbon-neutral fuels, but directing the multielectron pathway beyond the CO intermediate remains a central challenge. Here, by growing Pd nanoparticles in situ on oxygen-deficient TiO 2 (Pd/TiO 2-x ), we construct an oxygen-vacancy-rich Pd-O-Ti interface that functions as a CO-hydrogenation box. Interfacial oxygen vacancies enrich and retain CO 2 -derived carbon intermediates, whereas adjacent Pd sites promote H 2 O activation and provide reactive surface hydrogen species in the same nanoscale region. This spatial coupling of CO confinement and hydrogen delivery favors sequential C-H bond formation and suppresses premature CO desorption, thereby redirecting CO 2 photoreduction toward CH 4 . As a result, Pd/TiO 2-x achieves 100% CH 4 selectivity with a CH 4 production rate 40 times higher than that of TiO 2 under AM 1.5 G irradiation. Under natural sunlight, the catalyst delivers a CH 4 production rate of 1.1 mmol h −1 g −1 and sustained activity over repeated daytime cycles. These results identify an interfacial design principle for steering multielectron CO 2 photoreduction toward deeply reduced hydrocarbon products. Download: Download high-res image (199KB) Download: Download full-size image
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ADVANCED MATERIALS
·
2026
·
IF 29.1
Jiage Yu,Wei Liu,Lu Bai,Benqiang Tian,Qingyi Zhu,Qianxi Yang,Linlin Zhou,Haoyang Wu,Yuan Wang,Boyuan Li,Xiangrong Jin,Yun Kuang,Jiazhan Li,Xiaoming Sun
CO 2 electroreduction typically requires large overpotentials to sustain high reaction rates, which at current densities approaching 1 A cm −2 inevitably intensify competition from the hydrogen evolution reaction (HER), making it difficult to simultaneously sustain high product selectivity (>95%). In this study, hollow Ni─NC (H-Ni-NC) was synthesized using nanoscale silica sphere templates and atomic Zn as a sacrificial pore-former within the carbon shell. The optimized H-Ni-NC achieves a current density of −1.0 A cm −2 with over 95% CO Faradaic efficiency in a flow cell. The high performance was attributed to the hollow sphere architecture enriched with gas-permeable through-pores. Notably, the Zn dosage selectively modulates the shell through-porosity, without altering hollow sphere macrostructure or the active-site structure, thereby enabling a systematic investigation of porosity effects. Finite-element simulations provide a qualitative framework suggesting a trade-off between reactant transport and active surface area with increasing porosity in hollow spherical catalysts. This work underscores that engineering of the nanoscale mass-transport environment surrounding active sites plays a critical role in designing high-efficiency electrocatalysts.
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