CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Ruyang Song,Jinghong Wen,Hongji Liu,Wenjing Song,Chuanyue Sun,Bo Wang,Shuo Tao,Abdullah N. Alodhayb,Jinsheng Zhao,Zhou Chen,Xiaodong Yi,Yunyun Dong
The conversion of CO 2 to CO via the reverse water-gas shift (RWGS) reaction is crucial for CO 2 hydrogenation. However, conventional thermal catalysis relies heavily on fossil fuels and fails to achieve carbon neutrality. Photothermal catalysis offers a promising alternative pathway for efficient CO 2 conversion. Yet, enhancing CO 2 adsorption and activation for high activity and selectivity remains a challenge in RWGS reactions. In this article, a series of Ni supported catalysts (Ni/MgO -x , where x = 1.2, 2.4, and 3.6) with abundant oxygen vacancies (Ovs) were prepared using a simple combustion method with magnesium acetate (Mg(CH 3 COO) 2 ) and urea as precursors. The results indicate that Ni/MgO -x catalysts with higher Ovs concentrations exhibit enhanced efficiency compared to Ni/MgO catalysts. The optimized catalyst achieved a high CO yield rate (12 mmol g −1 h −1 ), which was 36 times greater than that of the control catalyst under 1 W cm −1 lamp irradiation at 300 °C. Detailed characterization and density functional theory (DFT) results revealed an HCOO* reaction pathway and demonstrated the role of excess Ovs in CO 2 adsorption, activation, and reduction of the RWGS reaction activation energy. This research explores novel approaches for RWGS based on MgO supports for efficient CO 2 adsorption and activation, coupled with low-temperature synergistic photothermal effects.
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Fuels
·
2025
·Vol. 6
·期 4
·76
·
IF 2.8
Jun Hu,Hongyang Yu,Yanan Wang
The chemical looping steam reforming of methane (CLSR) employing Fe-containing oxygen carriers can produce syngas and hydrogen simultaneously. However, Fe-based oxygen carriers exhibit low CH4activation ability and cyclic stability. In this work, oxygen carriers with fixed Fe content and different Fe/Ni ratios were synthesized by the sol–gel method to investigate the effects of Ni-Fe-Al interactions on CLSR performance. Ni-Fe-Al interactions promote the growth of the spinel structure and regulate both the catalytic sites and the available lattice oxygen, resulting in the CH4conversion and CO selectivity being maintained at 96–98% and above 98% for the most promising oxygen carrier, with an Fe2O3content of 20 wt% and Fe/Ni molar ratio of 10. The surface, phase, and particle size were kept the same over 90 cycles, leading to high stability. During the CLSR cycles, conversion from Fe3+to Fe2+/Fe0occurs, along with transformation between Ni2+in NiAl2O4and Ni0. Overall, the results demonstrate the feasibility of using spinel containing earth-abundant elements in CLSR and the importance of cooperation between oxygen release and CH4activation.
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Catalysts
·
2025
·Vol. 15
·期 6
·559
·
IF 4
Zhizhi Tao,Dong Shen,Yanni Liu,Xiaodi Zhang,Guojie Zhang
The dry reforming of methane (DRM) converts two greenhouse gases, CH4and CO2, into H2and CO, offering a crucial technological pathway for reducing greenhouse gas emissions and producing clean energy. However, the reaction faces two main challenges: high activation energy barriers require high temperatures to drive the reaction, while sintering and carbon deactivation at high temperatures are common with conventional nickel-based catalysts, which severely limit the further development of the methane dry reforming reaction. In this study, a nitrogen-doped carbon nanotube-loaded nickel catalytic system (Ni/NCNT) was developed to overcome the challenges caused by limited active sites while maintaining the stable structure of the Ni/CNT system. Ni/NCNT catalysts were prepared using different nitrogen precursors, and the impact of the mixing method on catalytic performance was examined. Characterization using H2-TPR, XPS, and TEM revealed that nitrogen doping enhanced the metal–support interaction (MSI). Additionally, pyridine nitrogen species synergistically interact with nickel particles, modulating the electronic environment on the carbon nanotube surface and increasing catalyst active site density. The Ni/NCNT-IU catalyst, prepared with impregnated urea, exhibited excellent stability, with methane conversion decreasing from 85.0% to 82.9% over 24 h of continuous reaction. This study supports the use of non-precious-metal carbon-based catalysts in high-temperature catalytic systems, which is strategically important for the industrialization of DRM and the development of decarbonized energy conversion.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2025
·
IF 8.3
Fang-Qing Zou,Ye Xiao,Chuan-Jin Tian,Yu-Min Liu,Wen-Yan Zhao,Chang-An Wang
Reasonably designing and optimizing the homogenous surfaces of catalysts with moderate noble metal loadings to enhance their electrolysis of water performance in alkaline environments has always been a challenge. In this work, we proposed a heterostructure induction technique employing Ru nanoparticles, Ni, and NiO to accurately produce a highly distributed three-phase heterostructure Ru@Ni/NiO, which exhibits excellent catalytic performance for oxygen evolution reaction (OER), hydrogen evolution reaction (HER), and overall water splitting reaction under alkaline conditions. The OER overpotentials in 1 M KOH were 250 mV, 320 mA, and 350 mV at 10 mA cm −2 , 50 mA cm −2 , and 100 mA cm −2 current densities, respectively, outperforming RuO 2 . The HER overpotentials were 52 mV, 107 mV, and 142 mV, respectively, superior to Pt/C. In the overall water splitting reaction, the Ru@Ni/NiO system requires only 1.63 V, 1.94 V and 2.08 V to achieve current densities of 10 mA cm −2 , 50 mA cm −2 and 100 mA cm −2 , respectively. Meanwhile, the catalyst exhibited excellent stability at high current density. This study provides a design strategy for the precise construction of interfacial engineering and demonstrates significant potential for large-scale hydrogen production via electrochemical water splitting.
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ACS Catalysis
·
2026
·
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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JOURNAL OF ALLOYS AND COMPOUNDS
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2026
·
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
·
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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ACS Applied Materials & Interfaces
·
2026
·
IF 7.8
Chenliang Ye,Wei Zheng,Zhiguo Wang,Hao Chen,Yu Zhang,Zhiye Cheng,Haonan Ye,Shaoxuan An,Miaolun Jiao
The oxygen evolution reaction (OER) is a crucial half-reaction in water electrolysis. Currently, the sluggish kinetics of the OER limit the efficiency of water electrolysis, making the development of advanced OER catalysts imperative. Herein, utilizing carbonized wood (CW) as a self-supporting conductive substrate, we synthesized ultrafine Ni3Fe@Ni core–shell nanoparticles featuring a surface Ni3Fe alloy on unalloyed Ni nanoparticles. Ni3Fe@Ni/CW exhibits a low overpotential of 290 mV at 100 mA cm–2 with excellent stability, outperforming Ni3Fe/CW, Ni/CW, and RuO2/CW. In an overall water splitting electrolyzer, Ni3Fe@Ni/CW delivers a low cell voltage of only 1.74 V at 100 mA cm–2 with outstanding long-term stability. This unique surface-interior heterostructure, where the unalloyed Ni nanoparticles modulate both the geometric configuration and d-band center of the surface Ni3Fe alloy, optimizes the adsorption energetics of oxygen intermediates. Accordingly, for both Ni3Fe/CW and Ni/CW, the rate-determining step (RDS) is the conversion of O* to OOH*. In contrast, the RDS for Ni3Fe@Ni/CW is the OOH* to O2 step with a significantly lower energy barrier, accounting for its excellent OER performance. This work highlights the immense potential of surface-interior engineering for the rational design of high-performance OER catalysts.
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