BIOELECTROCHEMISTRY
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2026
·
IF 4.9
Honggui Wang,Yang Liu,Liuxiu Peng,Ya Zhang
Efficiently reducing carbon dioxide (CO 2 ) to high-value organic chemicals in microbial electrosynthesis (MES) systems hinges on the electrochemical performance of electrode materials. This study increased the efficiency of CO 2 reduction to acetic and formic acids by creating a carbon felt (CF) cathode co-modified with nickel‑cobalt bimetallic oxide (NiCo 2 O 4 ) and carbon nanotubes (CNT) coupled with an enriched mixed microbial community derived from anaerobic sludge. Compared to NiCo 2 O 4 /CF and CF cathodes, the CNT-NiCo 2 O 4 /CF cathode increased acetate yield by 1.3- and 2.3-fold, and formate yield by 1.1- and 2.4-fold, respectively. Within 8 days, the system achieved 742.98 mg/L acetate and 566.37 mg/L formate. Performance gains stem from: (1) the synergistic effect of CNT and NiCo 2 O 4 , which increased electrode surface area and electron transfer efficiency; (2) enhanced hydrophilicity, which improved microbe-electrode interactions; and (3) the presence of Co/Ni ions, which boosted CF conductivity and the selective enrichment of electroactive microbes (e.g., Sporomusa and Cupidesulfovibrio ). This study provides an innovative strategy for developing high-performance MES electrode materials. Through the synergistic design of bimetallic oxides and nanocarbon materials, the conversion of CO 2 to acetic acid and formic acid was achieved, offering a feasible technical pathway toward carbon neutrality.
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JOURNAL OF SOLID STATE CHEMISTRY
·
2026
·
IF 3.2
Yating Jiang,Xinrui Chen,Xuanyu Chen,Weibin Zhang,Syed Awais Ahmad,Xiankui Lv
Solar-driven CO 2 reduction is often limited by slow surface reactions and large thermodynamic barriers. In this work, we activated the hidden reactivity of molybdenum disilicide (MoSi 2 ) through controlled nitrogen (N) doping. Instead of simple physical mixing, nitrogen incorporation triggers a clear rearrangement of the crystal structure, leading to the preferred exposure of the active (110) facets and an improvement in the porous framework. Comprehensive spectroscopic analyses combined with density functional theory (DFT) calculations reveal a synergistic electronic modulation mechanism. Crucially, the formation of electron-rich Mo centers significantly lowers the work function and establishes a robust electron reservoir. This configuration thermodynamically drives the rapid injection of photogenerated electrons into surface-adsorbed species, effectively reversing the rate-determining protonation step of CO 2 * to COOH* from an endergonic barrier to a spontaneous process. As a result, the optimized catalyst achieves a striking 34-fold increase in the CO production rate and reaches a CO to CH 4 selectivity of about 134. This study not only explains how activity is improved in non-oxide systems from several different aspects but also provides a clear and practical approach for designing future intermetallic photocatalysts by carefully tuning their energy bands and defect states.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2026
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IF 9.1
Chunyu Li,Min Zhang,Zhenjiang Li,Yujia Wang,Na Shi,Yanqi Shi,Yue Xu,Jiahui Ma,Haoyu Wang,Kai Guo
The development of catalyst that workable homogeneously in reaction and recoverable heterogeneously in separation remains a challenge. We designed functionalized cellulose featuring malononitrile carbanion ion pair as a bifunctional catalyst for the cycloaddition of CO₂ to epoxides (CCE) reactions. The malononitrile (MNH) group was regioselectively anchored on the C-6 position of the anhydrous glucose unit of the cellulose backbone (Cell-MNH), and subsequently deprotonated with 1,8-diazabicyclo[5.4.0]undec-7-ene (DBU) yielding catalyst Cell-[MN][DBUH], which exhibited excellent catalytic activity in CCE reactions of styrene oxide under conditions of 120 °C, 1.0 MPa, and 8 h, with catalyst loading of 1.5 mol%, achieving a yield of 93% and a selectivity of 94%. A bifunctional catalytic mechanism was proposed in which the carbanion attacked the CO₂ and the 1,8-diazabicyclo[5.4.0]undec-7-enium (DBUH) as an H-bond donor activated the epoxide. NMR titration experiments validated the role of DBUH in coordinating to epoxide through hydrogen bonding, and 13 C NMR spectra revealed a carbonate intermediate derived from malononitrile carbanion and CO 2 . The catalyst was homogeneous at 120 °C during the reaction but precipitated upon cooling due to the inter-chain attractions of the positive and negative ions, allowing easy filtration and recycling. The catalyst maintained robust by yields of 82%–97% and selectivity of 92%–99% through five recycles. This lignocellulose-based ion pair organocatalyst enables efficient homogeneous catalysis with heterogeneous recovery, offering potential design and broad applicability.
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Nature Communications
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2026
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IF 18.1
Kang Xiaofeng,Jiang Mingyu,Lv Jiarong,Liao Chen,Ding Xue,Wang Feng,Bai Shengjie,Liu Ya,Guo Liejin
Improvement of solar-to-chemical energy conversion in photocatalytic CO 2 reduction remains fundamentally constrained by insufficient utilization of solar energy, particularly low-energy photons. Here we report a nanoscale greenhouse structure (Bi@Fe 2 O 3 ) that enables cascaded utilization of full solar spectrum. The Bi nanocore primarily absorbs low-energy photons, generating localized nanoheating via non-radiative heating through localized surface plasmon resonance effects and energetic hot electrons. Meanwhile, the oxygen-vacancy-rich loose Fe 2 O 3 shell absorbs high-energy photons and serves as the catalytic bed, where injected hot electrons and confined heat synergistically promote CO 2 activation and deep hydrogenation. Benefiting from the interplay between photochemical and photothermal effects, the system achieves a CH 4 production rate of 273.81 μmol g –1 h –1 with 98.60% selectivity and an apparent quantum efficiency of 0.64% at 850 nm illumination without any external heating or sacrificial agents. This work paves a way for the efficient utilization of the entire solar spectrum.
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JOURNAL OF SOLID STATE CHEMISTRY
·
2026
·
IF 3.2
Dijun Zhou,Jianwen Wei,Xuequan Zou,Linlin Geng,Xiaobin Zhou,Lei Liao
Amine scrubbing, while mature for CO 2 capture, suffers from solvent volatility. To address this, we developed a novel solid adsorbent by incorporating low-volatility ionic liquids (ILs), [TEPA][NO 3 ] and [PEHA][NO 3 ], into a hierarchical UiO-66@SBA-15 composite (US). The growth of UiO-66 within the mesochannels of SBA-15 was facilitated by interactions between Zr 4+ and surface Si–OH groups. IL loading dramatically increased the density of amine-based CO 2 adsorption sites. The optimized adsorbent, US-T60, achieved a high CO 2 capacity of 4.73 mmol g -1 at 60 °C under 15% CO 2 /85% N 2 , which is 4.15 times that of the pristine US composite. It also exhibited excellent regeneration stability, retaining 93% of its initial capacity after five cycles. Kinetic analyses indicated a mixed physisorption-chemisorption process, well-described by the Avrami model. In-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) revealed that CO 2 capture proceeded via two pathways: the rapid formation of ammonium carbamate ion pairs under amine-rich conditions, and the formation of hydrogen-bonded carbamic acid when proton transfer was hindered. Combined with its high capacity, good stability, and tunable adsorption mechanism, this family of IL-incorporated hierarchical composites demonstrates promising potential for application in post-combustion flue gas CO 2 capture.
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Nature Communications
·
2026
·
IF 18.1
Lang Hu,Yun Yang,Jiamin Wang,Dongao Zhang,Jingya Huang,Yuqi Zhang,Xiaodong Yi,Guoxiong Wang,Zhou Chen
Electrocatalytic CO 2 reduction reaction (CO 2 RR) technology holds significant industrial potential. However, when faced with elevated-temperature environments caused by industrial-scale operations, the fundamental understanding of temperature-dependent CO 2 RR behavior in flow cells remains elusive. This study points out that elevated-temperature operation (>333 K) presents both challenges and opportunities for multi-carbon (C 2+ ) production. While elevated temperature enhances reaction kinetics and reduces thermodynamic energy barriers, it simultaneously induces reconstruction of Cu-based catalyst, accelerates gas diffusion electrode flooding, and promotes *CO desorption together with hydrogen evolution reaction, collectively suppressing C 2+ product formation and compromising long-term reactor stability. Through rational design of hydrophobic-enhanced Pd-Cu 2 O/polytetrafluoroethylene (PTFE)/Ag tandem electrodes, we overcome these challenges. Leveraging thermal reduced C-C coupling barriers, the optimized electrode achieves >70% Faradaic efficiency of C 2+ across industrially relevant current densities (200–1000 mA cm −2 ) at 348 K. This strategy converts elevated temperature adversity into a kinetic and thermodynamic advantage, boosting C 2+ cathodic energy efficiency by 1.3 times compared to ambient operation, establishing a promising paradigm for industrially viable CO 2 electrolysis. The electrocatalytic reduction of CO 2 offers industrial potential, but elevated temperatures hinder efficient production of valuable multi-carbon compounds. Here, the authors report a synergistic electrode design for efficient CO 2 electrolysis to multicarbon products at 348 K.
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CHEMICAL ENGINEERING SCIENCE
·
2026
·
IF 5.1
Hang Yao,Jian Sheng,Jie Fan,Hong-Mei Jiang
The selective hydrogenation of CO 2 to either CH 4 or CO is a pivotal reaction for sustainable chemical synthesis, yet controlling product selectivity remains challenging. Although Ru-based catalysts are highly active for CO 2 methanation, their selectivity to CO is typically low. Herein, we demonstrate that gallium oxide (GaO x ) serves as an efficient promoter for Ru/Al 2 O 3 catalysts, switching the dominant product in ambient-pressure CO 2 hydrogenation from ∼98% CH 4 to ∼92% CO. Comprehensive characterization reveals that GaO x engages in a strong electronic metal-support interaction with Ru, which facilitates electron transfer from Ru to Ga, generating electron-deficient Ru sites that weaken CO adsorption. In situ DRIFTS further demonstrates that Ga redirects the reaction pathway from a dual mechanism favoring CH 4 formation on Ru/Al 2 O 3 to a selective route producing CO via formate intermediate decomposition. This work provides fundamental insights into how oxide promoters can steer reaction pathways through electronic effects and offers a rational strategy for designing selective CO 2 hydrogenation catalysts.
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JOURNAL OF MEMBRANE SCIENCE
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2026
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IF 8.8
Yuting Zhang,Qian Sun,Bizi Yu,Weiwang Lim,Ayan Yao,Jingcheng Du,Yumo Fan,Xuan Ding,Daijun Meng,Wen He,Ji Ma,Jian Guan,Hongjun Zhang,Jiangtao Liu
Mixed matrix membranes (MMMs) incorporating metal-organic frameworks (MOFs) hold great promise for energy-efficient carbon capture, yet are fundamentally limited by interfacial defects and the ubiquitous permeability-selectivity trade-off. Herein, we propose a nanoconfinement strategy via in-situ interfacial polymerization to synthesize ultrathin MOF nanosheets and thus integrate them into PIM-1 matrix, a typical representative of polymers of intrinsic microporosity (PIMs), crafting a defect-free membrane. The meticulously designed MOFs, featuring synergistic amino functionalities and unsaturated Cu 2+ sites, endows the optimal membrane (PIM-MOF-1%) with exceptional CO 2 affinity and tailored molecular-sieving pathways. Consequently, it achieves a remarkable combination of high CO 2 permeability (5186 barrer) and CO 2 /N 2 selectivity (41), surpassing the 2019 Robeson upper bound. Impressively, this superiority persists under harsh conditions-exceeding the 2008 Robeson upper bound at 80 °C and sustaining high performance at 15 bar. Moreover, the membrane demonstrates exceptional long-term durability, preserving excellent separation performance, with CO 2 permeability of 3078 barrer and CO 2 /N 2 selectivity of 46, even after 180 days of aging. Our strategy aligns nanoconfined MOF architectures with polymer matrix, thereby resolving critical challenges in carbon capture through the simultaneous enhancement of separation efficiency and durability.
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JOURNAL OF CATALYSIS
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2026
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IF 6
Xinping Duan,Jinlin Lu,Zhaojun Wen,Xuelian Liang,Haiqiang Lin,Linmin Ye,Youzhu Yuan
In supported metal catalysis, conventional strong metal-support interaction (SMSI) often leads to the encapsulation of active metal sites, thereby suppressing catalytic performance, for instance, nickel-based in thermocatalytic CO 2 hydrogenation. Here, we demonstrate that constructing a defective TiO x overlayer on anatase TiO 2 via room-temperature NaBH 4 treatment effectively transforms the classical SMSI state into a quasi-reactive metal-support interaction (quasi-RMSI) in Ni/TiO 2 -based catalysts. This pre-engineered interface, abundant in Ti 3+ and oxygen vacancies, prevents the formation of a dense TiO x encapsulation layer while facilitating electron transfer to Ni nanoparticles and promoting the activation of both CO 2 and H 2 . As a result, the Ni catalyst exhibits a one-order-of-magnitude increase in the CO 2 methanation rate with nearly 100% CH 4 selectivity, a 12-fold enhancement in turnover frequency, and exceptional long-term stability over 200 h. Combined spectroscopic and microscopic analyses reveal that the quasi-RMSI creates a highly active and accessible Ni-TiO x interface, which significantly accelerates CO 2 dissociation and sequential hydrogenation. This work establishes a general defect-engineering strategy for designing high-performance CO 2 methanation catalysts via tailored quasi-RMSI.
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ACS Applied Nano Materials
·
2026
·Vol. 9
·期 29
·13860-13868
·
IF 5.8
Li Bingshuang,Li Xin,Huang Xiaoxi
The
electrochemical CO 2 reduction reaction (CO 2 RR)
to produce multicarbon products represents a promising route
for sustainable carbon utilization. Copper-based catalysts are unique
in catalyzing C–C coupling, but the active Cu + species,
which favor ethylene formation, are prone to reduction during reaction.
In this work, we demonstrate that halogen doping, combined with a
nanoconfinement strategy, effectively stabilizes Cu + within
a nanoporous carbon matrix. Two model catalysts supported on porous
carbon spheres (Cu@C-1 derived from CuCl 2 and Cu@C-2 from
CuSO 4 ) were synthesized. After calcination, Cu@C-1 predominantly
comprises CuCl while Cu@C-2 mainly consists of Cu 2 O with
trace sulfur doping. They both have a similar average copper oxidation
state. During the CO 2 RR at −1.3 V versus the RHE,
the Cu@C-1 nanocatalyst achieves selective ethylene production with
a Faradaic efficiency (FE) of 41.5% and a partial current density
of 110.7 mA cm –2 whereas the Cu@C-2 nanocatalyst
primarily generates methane (FE of 49.5% and partial current density
of 124.4 mA cm –2 ). In situ and postreaction characterizations
reveal that nanoscale confinement in Cu@C-1 maintains its CuCl phase
under the reaction conditions, which promotes the *COCHO intermediate
and facilitates C–C coupling toward ethylene. Conversely, Cu@C-2
nanoparticles are reduced to metallic Cu 0 , favoring the
methane pathway. This work highlights that tailoring the precursor
anion offers a precise level of control over the initial copper phase
and its dynamic state under electrolysis, thereby steering the CO 2 RR selectivity toward the desired products.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2026
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IF 19.7
Boyang Zhang,Zhiyong Zhang,Yangfan Li,Yangqi Wei,Xingmiao Huang,Chuncheng Chen,Hua Sheng,Jincai Zhao
Post-synthetic strategy modularly integrates CO 2 -to-CO and CO-to-C 2+ sites. • Redox mediator and confinement synergize to regulate cascade reactions. • Confined TEMPOL acts as PCET mediator, lowering CO 2 -to-*COOH barrier. • Inactive MOF is transformed into an efficient CO 2 -to-C 2+ electrocatalyst. Efficient electrochemical conversion of CO 2 to multi-carbon (C 2+ ) products requires the integration of two sequential functionalities: CO 2 activation to *CO and subsequent CO-initiated C-C coupling. Conventional strategies typically rely on the rigid, pre-designed incorporation of these two functional units during catalyst synthesis. In contrast, we propose a post-synthetic modification strategy that introduces a molecular CO 2 activation unit into a pre-formed catalyst scaffold, thereby enabling its spatially proximal coupling with intrinsic CO reduction sites. This concept is demonstrated by encapsulating 4-hydroxy-2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPOL) into the pores of a tetrapyrazolylporphyrin copper-based metal–organic framework (FICN-8). Owing to the well-matched molecular dimensions, the confined TEMPOL and adjacent Cu nodes cooperatively define a cavity that spatially accommodates a CO 2 molecule. Reduced TEMPOL acts as a proton-coupled electron transfer (PCET) mediator, while spatial confinement regulates the local reaction environment, jointly lowering the free energy barrier for *COOH formation. The confined *COOH intermediate is subsequently converted to CO and further undergoes C–C coupling. As a result, FICN-8—originally inactive for CO 2 -to-C 2+ conversion (Faradaic Efficiency, FE< 0.6%)—is transformed into an efficient electrocatalyst, delivering a C 2+ Faradaic efficiency of 42.6% with a two-orders-of-magnitude enhancement in C 2 H 4 formation rate. Download: Download high-res image (123KB) Download: Download full-size image
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2026
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IF 3.5
Chaoyue Zhang,Mingrui Wang,Xinyue Han,Zheng Shen,Hongying Zhuo,Tianyu Zhang,Xiaofeng Yang,Yanqiang Huang
Metastable hcp-Ni enables the synthesis of highly dispersed and stable Ni/Al 2 O 3 catalyst • Highly dispersed Ni/Al 2 O 3 catalyst delivers 75.7% CO 2 conversion and 100-h stability • Original hcp-Ni particles spontaneously transform into fcc-Ni clusters of ∼2.3 nm • Small Ni clusters promote CO 2 methanation via monodentate formate intermediate • Fcc-Ni precursors undergo severe sintering to ultra-large and less-active particles Ni-based catalysts are promising candidates for CO 2 methanation while their practical applications are limited by particle agglomeration and deactivation. Here, we report a facile strategy to fabricate a highly dispersed and stable Ni/Al 2 O 3 catalyst using metastable hexagonal close-packed (hcp)-Ni as a precursor. Comprehensive characterization reveals that the initial hcp-Ni (∼12.0 nm) spontaneously transforms into uniform face-centered cubic (fcc)-Ni nanoparticles (NPs) of ∼2.3 nm on γ -Al 2 O 3 support during H 2 reduction and CO 2 methanation reaction. The small Ni particles contribute to improved Ni 0 proportion on catalyst surface. In contrast, the original fcc-Ni precursors are prone to sintering, forming ultra-large and less-active Ni aggregates. The highly dispersed Ni NPs derived from hcp-Ni enhance CO 2 adsorption-activation and facilitate the formate-mediated reaction pathway. The resulting hcp-Ni/Al 2 O 3 catalyst delivers a CO 2 conversion of 58.2% with a CH 4 selectivity of 85.4% at 460 °C and endows robust stability exceeding 100 hours. The optimal CH 4 space time yield reaches 179.5 mmol·g cat −1 ·h −1 , exceeding 2.4 times that of fcc-Ni/Al 2 O 3 . This work establishes a reliable synthesis paradigm rooted in crystal-phase regulation, enabling the manufacture of highly dispersed and stable Ni-based catalysts for efficient CO 2 methanation. Manufacturing Highly Dispersed and Stable Ni/Al 2 O 3 Catalysts from hcp-Ni for Enhanced CO 2 Methanation Download: Download high-res image (221KB) Download: Download full-size image
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