ACS Catalysis
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2026
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IF 13.1
Wendong Wang,Xingwen Cha,Longmei Shang,Kang Sun,Fangsong Guo,Jianchun Jiang,Guowu Zhan
This work demonstrates a strategic shift from dynamic electrolyte modulation to static, intrinsic promotion of the CO2 reduction reaction by stably integrating alkali metal cations as a solid-state component within a heterogeneous catalyst. To address the persistent challenge of alkali metal ion leaching due to high aqueous solubility, we immobilize K+ cations into a carbon nitride framework (Ni@K–C3N4) hosting atomically dispersed Ni–N3 sites via an ionothermal strategy. Structural confinement through coordination with nitrogen sites in the C3N4 matrix effectively suppresses K+ leaching, enabling sustained electronic regulation of the Ni centers. Combined experimental and theoretical analyses reveal that K+ incorporation attenuates d-π conjugation, promotes electron localization around Ni sites, and stabilizes low-valent Niδ+ species. This electronic reconfiguration enhances CO2 adsorption and activation while suppressing competitive hydrogen evolution reaction. The optimized Ni@K–C3N4 catalyst achieves a CO Faradaic efficiency of 95% at −0.74 V vs RHE, a current density of ∼20 mA·cm–2, and stable operation over 50 h. Notably, it maintains >80% CO selectivity under a diluted CO2 atmosphere (40%), highlighting its practicality for real low-concentration streams. This work establishes a polymer-functionalization strategy for precise electronic tuning of single-atom catalysis, advancing the design of efficient CO2 utilization systems.
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ACS Catalysis
·
2026
·
IF 13.6
Shuangfeng Ren,Yihui Li,Ye Chen,Xiaoling Mou,Ziang Zhao,Hejun Zhu,Xiaoyan Liu,Yu Meng,Li Yan,Apoorva Ravi,Amol Amrute,Ronghe Lin,Yunjie Ding
The rational design of selective, earth-abundant Ni-based catalysts for the reverse water–gas shift (RWGS) reaction is often hampered by an incomplete understanding of their operando active states. This study reveals that the CO2 hydrogenation selectivity over Ni–Zn catalysts is governed by a support-dependent, reaction-induced dynamic restructuring, rather than by any static, preformed sites. Through a combination of in situ characterization and theoretical calculations, we demonstrate that the active Ni–Zn intermetallic core encapsulated by ZnO forms dynamically only under the RWGS atmosphere on ZrO2 and TiO2 supports, but not on Al2O3 or during mere H2 reduction. Crucially, we identify in situ-generated CO as the essential inducer of this reconstruction, likely via facilitating ZnO reduction. Furthermore, the product selectivity (CO vs CH4) is dictated by the kinetic competition between CO desorption and its deep hydrogenation, a principle quantitatively linked to the evolved electronic structure of the active surface. This work shifts the paradigm toward designing catalysts that evolve into optimal structures in operando and provides a fundamental kinetic framework for selective CO2 conversion.
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CHEMICAL ENGINEERING SCIENCE
·
2026
·
IF 5.1
Tianhao Zhang,Junjie Fan,Xinyu Yuan,Jianwen Hu,Haotian Gao,Wenqing Xie,Jingwen Wang,Jian Yang,Chunling Li,Shuangqing Sun
This study presents a novel responsive carbon dot-based surfactant system that exhibits catalytic activity at the interface of an oil-in-water Pickering emulsion microreactor containing reactants. Nickel nitrate was employed to dope carbon dots via a microwave-assisted method, imparting catalytic functionality to the resulting nanomaterials. Subsequently, poly[2-(dimethylamino)ethyl methacrylate] (PDMAEMA) was grafted onto the surface of the nickel-doped carbon dots through electron transfer radical polymerization, yielding the catalytically responsive solid emulsifier Ni@CD-NH-Met-PDMAEMA (Ni@CD-3). Owing to the metal doping of carbon dots and subsequent emulsification functionalization, Ni@CD-3 demonstrates exceptional ability to stabilize reactive droplets in Pickering emulsion while exhibiting intrinsic catalytic activity at the oil–water interface. Notably, Ni@CD-3 exhibits high catalytic activity, with an extremely short reduction reaction time required to achieve a conversion efficiency exceeding 99%, attributed to the advantageous interfacial properties of the emulsion. Its catalytic efficiency is 560% higher than that of Fe@CD-3 under comparable conditions. Furthermore, the cyclic response property of Ni@CD-3 enables in situ separation and emulsion-breaking recovery by adjusting the pH at the end of the reaction. This property facilitates the recovery and reuse of the catalyst for up to five cycles, with the catalytic efficiency maintained above 99% for the first three cycles. These results suggest that the Ni@CD-3-based emulsion microreactor system holds great promise as a high-performance catalyst for diverse organic chemical reactions.
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CHEMICAL ENGINEERING SCIENCE
·
2026
·
IF 5.1
Chaoran He,Shanshan Zhao,Jiafei Lyu,Bofeng Zhang,Rongrong Zhang,Guozhu Liu
The severe carbon deposition that plagues conventional Ni catalysts in dry reforming of methane (DRM) originates from the kinetic mismatch between CH 4 cracking and CO 2 dissociation. Here, we design an atomically thin Sm-doped MgAlO x overlayer to encapsulate Ni nanoparticles, creating a confined reaction environment that intrinsically couples these two critical steps. The Sm-induced electron donation to Ni accelerates CH 4 dissociation by weakening the C-H bonds, while the Sm-doped thin overlayer with rich oxygen vacancies facilitates the rapid decomposition of CO 2 -derived carbonate intermediates (m-CO 3 2− ) and shortens the diffusion path for the resultant active oxygen species to gasify surface cavrbon precursors. The optimized catalyst achieves high conversions of CH 4 (91.0%) and CO 2 (94.0%) at 800 °C, reducing carbon deposition from 39.47% to 9.50%, and maintains stable performance over 100 h. This work demonstrates that precise reducible-oxide overlayers engineering can intrinsically align reaction kinetics to break the classical deactivation cycle of Ni-based catalysts in DRM.
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CHEMICAL ENGINEERING SCIENCE
·
2026
·
IF 5.1
Wenlong Gao,Jinpeng Wei,Yonggang Sun,Yuyu Wang,Feng Lin,Yulong Ma
A composite catalyst that combines acid and metal catalysis has been developed. • Selectivity of up to 83.12 % toward MAHs achieved in lignin pyrolysis. • Heating rate affects routes and activation energy in catalytic lignin conversion. • SiW affords B acid sites while Ni centers stabilize intermediates and inhibit coking. To address the challenges of complex deoxygenation pathways and low monoaromatic hydrocarbon (MAHs) selectivity in the catalytic conversion of lignin, a series of SiW/Ni-MCM-41 metal–acid bifunctional catalysts were synthesized via an incipient wetness impregnation method. The effects of silicotungstic acid (SiW) loading ratios on the physicochemical properties of the catalysts and their performance in lignin catalytic pyrolysis were systematically investigated. Characterization results revealed that both SiW and Ni species were highly dispersed on the surface of the MCM-41 support, with interactions between them. With increasing SiW loading, specific surface area and pore volume decreased, Brønsted acid proportion increased, and total acid sites decreased mainly due to Lewis acid loss, enabling Brønsted/Lewis acid balance tuning. Catalytic performance evaluation demonstrated that the catalyst with a SiW-to-Ni-MCM-41 mass ratio of 1:2 exhibited the optimal lignin conversion (80.25 %) and MAHs selectivity (83.12 %), alongside excellent universality in substrate extension experiments. Kinetic analysis indicated that the apparent activation energy is heating-program dependent. In-situ FTIR confirmed that the Brønsted acid sites provided by SiW promoted deoxygenation and alkylation reactions, the Ni metal centers assisted deoxygenation and stabilized the aromatic ring structure via hydrogen-transfer-related pathways, while inhibiting condensation and coking side reactions to a certain extent; and the mesoporous MCM-41 framework provided a highly dispersed environment and a possible confinement-like effect, collectively driving the efficient conversion of lignin into monoaromatic hydrocarbons. This study provides a novel design strategy for metal–acid synergistic catalysts in the field of high-value conversion of lignin. Download: Download high-res image (144KB) Download: Download full-size image
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2026
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IF 19.7
Xiaoxue Zhang,Ru Jia,Zhen-Feng Huang,Lun Pan,Chengxiang Shi,Xiangwen Zhang,Guidong Yang,Ji-Jun Zou
Ni-doped Cu nanowires catalyst enables Cu sites to activate NO and Ni sites to accelerate water dissociation to supply *H. • In situ tests confirm Ni doping reduces charge transfer resistance, accelerates the Volmer step, and increases *H coverage. • CuNi 10% NWs catalyst has industrial-scale current density (>1000 mA cm −2 ) and 90.35% NH 3 Faradaic efficiency in a flow cell. • CuNi 10% NWs catalyst achieves 82.47% NH 3 Faradaic efficiency in a membrane electrode assembly with excellent stability. The electrocatalytic nitric oxide reduction reaction (NORR) presents a promising method for simultaneously mitigating nitric oxide (NO) pollution and synthesizing ammonia (NH 3 ). However, its practical application is hindered by sluggish kinetics, primarily due to inefficient water dissociation, which results in an inadequate supply of active hydrogen (*H) and thereby limits the hydrogenation of nitrogen-containing intermediates. Herein, we present Ni-doped Cu nanowires as a high-performance electrocatalyst for the NORR. The optimized catalyst with a Ni/(Ni + Cu) molar ratio of 10% (CuNi 10% NWs) delivers an industrial-scale current density exceeding 1000 mA cm −2 in a flow cell, achieving an exceptional Faradaic efficiency (FE) of 90.35% and an NH 3 yield rate of 6.84 mmol h −1 cm −2 (17.28 mmol g cat −1 h −1 ) at −1.0 V vs. reversible hydrogen electrode. Furthermore, in a membrane electrode assembly, the CuNi 10% NWs achieved an NH 3 FE of 82.47% and an NH 3 yield rate of 4.44 mmol h −1 cm −2 (8.88 mmol g cat −1 h −1 ). Remarkably, in situ electrochemical impedance spectroscopy and Tafel slope analyses reveal that Ni doping reduces the interfacial charge transfer resistance of Cu nanowires, accelerates the rate-determining Volmer step of water dissociation, and facilitates the generation and adsorption of *H intermediates. This study opens a new pathway for the resource utilization of industrial waste gas NO and the direct synthesis of NH 3 . Download: Download high-res image (156KB) Download: Download full-size image Ni-doped Cu nanowires catalyst acts as a high-efficiency catalyst for electrocatalytic NO-to-NH 3 conversion, where Cu sites activate NO and Ni sites accelerate water dissociation to enrich active hydrogen species, thus achieving superior catalytic activity for NH 3 synthesis.
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CHEMICAL ENGINEERING SCIENCE
·
2026
·
IF 5.1
Yu Shi,Fagen Wang
Ni/SiC catalysts were developed for low-temperature microwave-assisted DRM. • The interaction between microwave and Ni/SiC catalyst were revealed. • Ni/SiC interfacial polarization enhances DRM over conventional thermal. • Reactive intermediates (CH x O*, COOH*) were identified in microwave-assisted DRM. • Ea of CH 4 and CO 2 were decreased under microwave irradiation condition. Dry reforming of methane (DRM) reduces CH 4 and CO 2 emissions by producing syngas. Conventional thermal DRM requires temperatures above 973 K, leading to Ni sintering and carbon deposition. Developing Ni catalysts with high conversion at lower temperatures remains challenging. In this work, we developed Ni/SiC catalysts to investigate DRM under microwave irradiation conditions below 973 K. The Ni/SiC catalysts markedly enhanced performance of low-temperature DRM by microwave catalysis compared to conventional thermal catalysis. The comprehensive characterizations, including physicochemical properties, microwave adsorption properties, and in-situ DRIFTS, reveal that the performance enhancements are primarily attributed to interfacial polarization on the Ni-SiC surface, which generates microcurrent facilitating the formation of reactive intermediates (CH x O*, COOH*) and reducing the activation energies of CH 4 and CO 2 . The work highlights the significance of interfacial polarization on Ni/SiC catalysts in enhancing DRM performance, and the polarization strategy can be applied to other reactions under microwave irradiation conditions. Download: Download high-res image (223KB) Download: Download full-size image
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CERAMICS INTERNATIONAL
·
2026
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IF 6
Tao Wen,Xiaoyan Yang,Yanwei Yuan,Xiaoke Lv,Zhen Wang,Tianmeng Zhang,Bin Wu,Jianjun Chen
With the widespread proliferation of electronic and intelligent devices, increasingly stringent requirements have been imposed on microwave absorption materials. Ti 3 C 2 T x MXene is considered a promising microwave absorbing material with excellent properties. However, its high electrical conductivity and monotonous loss mechanism restrict its development in the field of microwave absorption. In this work, Ti 3 C 2 T x /Ni-Fe Prussian blue analogue (PBA) porous composites were synthesized via ion intercalation and chemical synthesis methods. The hollow cage-like Ni-Fe PBA was in-situ grown between the Ti 3 C 2 T x nanosheets. Benefiting from the magnetic loss characteristics and porous structure of Ni-Fe PBA, both the magnetic loss and polarization loss of Ti 3 C 2 T x were enhanced. The synergistic effect of multiple loss mechanisms optimized the impedance matching. Furthermore, the hollow cage-like structure of Ni-Fe PBA extended the propagation path and prolonged the transmission time of incident electromagnetic waves, thereby significantly improving the microwave absorption performance of the composite material. Consequently, the Ti 3 C 2 T x /Ni-Fe PBA composites achieve a significantly improved minimum reflection loss (RL min ) of −48.97 dB and an effective absorption bandwidth (EAB) of 3 GHz at a thickness of 3.9 mm. The radar stealth performance of the composite was evaluated by radar cross-section (RCS) simulation, with the maximum RCS reduction value reaching 11.75 dB m 2 . This work provides a promising strategy for developing high-performance microwave absorbers through structural and compositional design.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2026
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IF 6.7
Chao Chen,Meng-Han Li,Ya-Yun Ma,Guo-Zhi Han
Photo-deposition method has the advantages of simplicity, environmental friendliness, and high efficiency, and has been widely used in the field of materials preparation. In this paper, we firstly prepared hollow black TiO 2 microspheres by template method, then using the mesoporous hollow microspheres as a carrier, NiCl 2 ·6 H 2 O as raw material, a novel kind of hollow Ni(OH) 2 @TiO 2 composite microspheres was prepared by photochemical deposition. Characterization of X-ray diffraction (XRD), transmission electron microscopy (TEM), scanning electron microscopy (SEM), fluorescence spectrophotometry (PL), X-ray photoelectron spectroscopy (XPS), and Fourier transform infrared spectroscopy (FT-IR) indicated that the two units of TiO 2 and Ni(OH) 2 in the composite hollow microspheres form tightly chemical connections. More importantly, this chemical connection endowed the two functional units with mutually enhanced catalytic performance for reduction of aromatic nitro compounds and photocatalytic degradation of emerging organic pollutants. For example, it can catalyze the reduction of 4-nitrophenol (4-NP) to 4-aminophenol (4-AP) by NaBH 4 with a k value of 0.8457 min −1 , as well as degrade tetracycline hydrochloride (TCH) with a degradation rate of 92.29% within 60 min with a k value of 0.0606 min −1 , which is superior to most previous reports. Finally, based on a series of control experiments, a plausible mutually enhanced catalytic mechanism was proposed.
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SENSORS AND ACTUATORS B-CHEMICAL
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2026
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IF 8.3
Jingyi Yang,Yong Zhang,Zhiheng Ma,Jiaqiang Xu,Chenglin Sun
The development of highly selective trace ammonia (NH 3 ) detection technology based on metal-organic frameworks (MOFs) is of critical significance for the precise monitoring of ammonia in industrial and agricultural production environments. In this study, a series of UiO-66 materials doped with different metal ions (X-UiO-66, X = nickel, copper, iron, and aluminum) were synthesized. Through comparative analysis, the Ni-UiO-66 based QCM sensor exhibited superior sensing performance for trace NH 3 at room temperature: A detection limit as low as 50 ppb, high sensitivity (frequency response of 1766 Hz to 25 ppm NH 3 ), fast response/recovery times (10 s/13 s), as well as good selectivity, long-term stability, and reliable detection capability in high-humidity environments. The doping of Ni 2 + creates defects in the framework, increases the specific surface area, and provides more abundant active adsorption sites, thereby significantly enhancing the sensitivity to NH 3 . Furthermore, adsorption tests, Gaussian simulations, and in-situ infrared spectroscopy revealed a significantly optimized reversible weak chemical adsorption interaction between Ni-UiO-66 and NH 3 , which endowed the material with enhanced selectivity compared to pristine UiO-66 toward NH 3 . This work provides a reliable strategy for designing MOF-based sensing materials that combine structural stability and high activity.
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MICROCHEMICAL JOURNAL
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2026
·
IF 5.2
Shu-Yu Wang,Yin-Hong Niu,Fang-Di Hu
A ratiometric colorimetric sensing platform was developed for nitrite detection, featuring a trimetallic metal-framework (MOF) nanozyme (Mn/Ni/Fe-MOF) synthesized via a facile one-pot solvothermal method. Comprehensive characterization revealed its successful fabrication and superior structural properties. The rational design of the trimetallic system creates a synergistic electron transfer network, endowing it with significantly enhanced peroxidase-like activity that surpasses its mono- (Fe-MOF) and bimetallic counterparts (Mn/Fe -MOF and Ni/Fe -MOF). This advancement leads to a low detection limit of 1.39 μM and a wide linear range of 2.0–150 μM for nitrite sensing, improving the sensitivity of nanozyme-based colorimetric method. Leveraging this high activity, Mn/Ni/Fe-MOF catalyzed H 2 O 2 -mediated oxidation of colorless 3,3′,5,5′-tetramethylbenzidine (TMB) to blue product (oxTMB). Subsequently, a robust ratiometric platform (A 450 /A 652 ) was constructed based on a specific diazotization reaction between nitrite and oxTMB, which induced a distinct color change and an absorbance shift. Unlike single-signal assays prone to fluctuations, this internal reference mechanism automatically corrects for common interferences, ensuring high accuracy and reliability in complex matrices, as evidenced by excellent recoveries (97.9%–102.3%) in real samples (tap water and sausage). The entire system is characterized by remarkable simplicity: the nanozyme is synthesized via a facile one-pot method, and the detection requires only a single-step addition of nitrite to the pre-formed oxTMB system under mild acidic condition. This streamlined, “mix-and-detect” protocol avoids complex modifications, multi-step reactions, or sophisticated instruments, offering practical advantages for potential on-site application. This work presents a reliable, high-performance sensing strategy and highlights the great potential of multi-metal MOF nanozymes in designing advanced sensors.
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Nature Communications
·
2026
·Vol. 17
·期 1
·2333
·
IF 18.1
Xiao Tingjiao,Fang Zhen,Ran Nian,Liu Ronghui,Gao Yuxuan,Wu Jianbo,Liu Jianjun,Wang Hua,Lin Wen-Feng,Zhou Wei
Sluggish kinetics caused by 16-electron transfer hinders development of wide-temperature-range sodium-sulfur batteries. Here we report Sn-doped CoNiS multipods with an amorphous-crystalline interwoven structure. Employed as a positive electrode catalyst, the resulting sodium–sulfur battery exhibits a discharge capacity of 1320.8 mAh g −1 at 3 A g −1 after 1200 cycles at room temperature, together with stable and high-capacity electrochemical performance ranged from −20 to 50 °C. It has been evidenced that the amorphous/crystalline interfaces generated by Sn doping can adjust the microelectronic environment of Co and Ni atoms, optimize their adsorption energy toward sodium polysulfide intermediates through Co–S and Ni–S bonding, and thus decrease the energy barrier of polysulfide conversion. This interfacial regulation efficiently lowers the energy barrier of the rate-determining step and facilitates the overall reaction kinetics over a wide temperature range. This work provides an efficient amorphous/crystalline interface engineering strategy to develop high-performance catalysts.
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