ACS Catalysis
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2024
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IF 11.3
Yanmei Cai,Cunbiao Lin,Xingwen Cha,Yiling Wu,Xiaoping Rao,Kok Bing Tan,Dongren Cai,Gui-Lin Zhuang,Guowu Zhan
The supported Ni/In2O3 catalysts are of great interest in CO2 hydrogenation, but the formation of the In0 or Ni–In alloy phases due to over-reduction would lead to rapid catalyst deactivation. Herein, thin Al2O3 films were deposited on the Ni/In2O3 surface by atomic layer deposition (ALD) as an antireduction agent, which enables the In2O3 catalyst to maintain a significant abundance of active In3+ species even during high-temperature H2 treatment (400 °C, 2 h), thereby effectively resisting the deactivation caused by over-reduction of In2O3. Various characterization methods confirm the antiover-reduction effect of ALD-Al2O3 films, namely, inhibiting the formation of In0 and In3Ni2 alloys during high-temperature H2 treatment and facilitating the reoxidation of low-valence In to form the active In2O3–x phase in the presence of a CO2 atmosphere. As treated with H2 at 400 °C, the 5Al2O3/Ni/In2O3-R400 catalyst exhibited an STYMeOH of 7.39 gMeOH h–1gNi–1 and a methanol selectivity of 64% (reaction conditions: 3 MPa, 300 °C, and 12,000 mL gcat–1h–1). Particularly, the STYMeOH increased by 11.5 times as compared with that of the Ni/In2O3-R400 catalyst without coating the ALD-Al2O3 layer (0.59 gMeOH h–1gNi–1). Density functional theory (DFT) calculations validate the effectiveness of specific charge transfer tendencies in suppressing the over-reduction of high-valence In species. Through the analysis of the crystal orbital Hamilton population (COHP) and projected density of states (PDOS) electronic structures of the adsorbate species, the Al2O3/Ni/In2O3 catalyst is shown to significantly enhance CO2 activation and further catalytic reactions. Accordingly, this study unveils the deactivation mechanism of In2O3-based catalysts due to over-reduction and provides a method to regulate their reduction level by depositing ALD-Al2O3 films on the In2O3-based catalysts.
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Chem Catalysis
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2024
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IF 11.5
Bin Chen,Shui Yang,Longmei Shang,Yiling Wu,Youting Wang,Jian Tian,Jiale Huang,Xiaodong Zhang,Qingbiao Li,Guowu Zhan
Biomass resources can be converted to biochemicals via the catalytic pyrolysis process, but conventional catalysts often suffer from severe deactivation due to coke formation. Here, a ternary Ni/bio-Z5 catalyst was constructed by integrating ZSM-5 and Ni components on a porous bio-SiO2 platform derived from rice husk. The Ni/bio-Z5 achieved 76% aromatic selectivity for the catalytic pyrolysis of soybean oil, corresponding to a space-time yield as high as 154.8 garom · h−1 · gcata−1. It is confirmed that the bio-SiO2 platform shortened the surface diffusion path of aromatics by co-diffusion, which then inhibited coke formation and significantly improved the catalyst stability. Moreover, the atomically dispersed Ni on ZSM-5 effectively promotes the aromatization of C2=-C6= by enhancing adsorption and acting as an oligomerization center for isoalkyl carbenium ions. The coupling of deoxygenation and aromatization reactions promotes the enhancement of aromatic selectivity through the formation of methyl-substituted cyclopentenone that can be readily converted to aromatics.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Shu-Xiang Xiang,Jin-Peng Wang,Su Gao,Zhan-Kuo Guo,Hui-Lin Jiang,Bao-Xia Dong,Yun-Lei Teng
The CH 4 yield over dual functional materials (DFMs) remains low and requires further improvement. In this work, we first examined the influence of Mn on the performance of the Ni-CaO/γ-Al 2 O 3 DFM for CO 2 capture and in situ methanation. Our results showed that the MnNi-DFM-3 (MnNi-CaO/γ-Al 2 O 3 DFM) exhibited the best performance at 350 °C, with a CH 4 yield of 0.56 mmol/g which is 4 times higher than that of the Ni-DFM-1 (Ni-CaO/γ-Al 2 O 3 DFM) (0.14 mmol/g). Nanoscale characterization revealed that highly scattered Mn 3 O 4 acted as a barrier preventing the agglomeration of Ni-based catalysts. Furthermore, our density functional theory (DFT) analysis demonstrated that the introduction of Mn enhanced the activation of CO 2 , promoted the dissociation of H 2 and intermediates, and reduced the activation energy needed to produce carboxylic acid intermediates on the Ni catalyst. The prepared MnNi-DFM is promising to be a cheap efficient material for CO 2 capture and in situ methanation. This work opens up a new pathway for enhancing the performance of DFMs using inexpensive transition metals.
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INTERNATIONAL JOURNAL OF ENVIRONMENTAL ANALYTICAL CHEMISTRY
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2025
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IF 2.5
Yuge Liu,Zhiguo Li,Yongmei Jia
The fast detection of environmental contaminants catechol (CC) and hydroquinone (HQ) is of great importance to public health. In this research, a composite was firstly synthesised by a pre-exfoliation method, the components of which were Ni-Al-LDH and reduced graphene (rGO). This material was then utilised in the development of a highly sensitive biosensor for determining CC and HQ. The construction procedure involved modification of glassy carbon electrode (GCE) by the composite and laccase (LAC). Tests conducted by electrochemical methods showed the addition of laccase can greatly improve the response signal of electrochemical measurements on the composite modified GCE to CC and HQ. The electrochemical tests were performed by utilising 0.1 mol/L phosphate-buffer. When separately detected, the detecting linear range for CC by the biosensor was 0.009–0.58 and 0.95–4.4 mmol/L. When it comes to HQ, the range was 0.009–0.57 and 0.95–4.4 mmol/L on the composite/enzyme modified electrode. When the biosensor was used for detecting CC and HQ together, the linear ranges were both 0.019–0.56 and 1.0–4.4 mmol/L. The detection limits calculated for simultaneous detection were 0.75 and 0.47 μmol/L, respectively. The sensor also possessed excellent sensitivity, selectivity and long stability. For applicability of the biosensor, it was used in analysing the two substrates in real water samples, and the recoveries were acceptable.
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Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Zhen-Qiang Yu,Yao-Xin Xiao,Dong Liang,Che Zhao,Zhen Huang,Gang-Qi Cheng,Rui Shan,Hao-Ran Yuan,Yong Chen
The chemical upgrade of the waste polyester coating on the surface of aluminum cans to value-added products can not only decrease the release of toxic substances, but also improve the quality of aluminum in the recycling process. In this study, different types of zeolite molecular sieve catalysts loaded with Ni, Mo and Co were synthesized, and utilized in the rapid catalytic pyrolysis of polyester coating. Among them, the Ni/ZSM-5 achieved the maximum aromatic compounds yield of 68.43 % at 600 ℃. A series of characterization results demonstrated that the embedding of transition metals (like Ni) could promote the cyclization and aromatization of products through deoxidation and dehydrogenation reactions by changing the pore structure and increasing total acid content (Brønsted and Lewis acids) of the ZSM-5 molecular sieve. Meanwhile, the thermodynamics of polyester coating during catalytic pyrolysis was studied by thermogravimetric method. The average activation energy of Ni/ZSM-5 catalytic pyrolysis of polyester coating is 238.65 kJ/mol. Furthermore, even after being reused for over 5 cycles, the catalyst can still maintain a relatively high yield of aromatic compounds (exceeding 60 %). Finally, the mechanism for aromatic compounds formation from Ni-modified ZSM-5 in-situ catalyzed polyester coating pyrolysis was proposed. This work provided useful ideas for the subsequent treatment of solid wastes.
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Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Liudi Ji,Fei Li,Qi Jia,Yicheng Yao,Xiaoming Zhu,Zeyu Li,Peng Hu
Developing rapid and reliable electrochemical monitoring methods for 4-CP is of great significance to ensure the safety of the water environment. Electrochemical sensing materials with high sensitivity and selectivity are urgently needed. Here, interlaced sheet-like Ni-BDC frameworks (BDC: 1,4-dicarboxybenzene) and multi-walled carbon nanotubes (MWCNTs) composite (Ni-BDC/MWCNTs) are constructed via in-situ self-assembly of Ni-BDC in the presence of MWCNTs at room temperature . Because of the large specific surface area , high electrochemical activity of Ni-BDC, and the outstanding electrical conductivity of MWCNTs, the obtained Ni-BDC/MWCNTs compound had a significant signal enhancement effect for the oxidation of 4-CP based on the large electrochemical active area, fast electron transfer ability, strong accumulation ability, and high electrocatalytic rate. It was found that the electrochemical oxidation of 4-CP involved the transfer of an electron and a proton. A wide linear range (0.1–50 and 50–500 μM), low detection limit (16.5 nM), high reproducibility, strong stability, and good selectivity were achieved at the Ni-BDC/MWCNTs sensing platform. It also has been successfully used to monitor 4-CP in different river water samples, and got similar results compared to HPLC, which provides promising potential for application in water environment safety monitoring and protection.
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Science China-Materials
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2024
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IF 6.8
Zhang Baichao,Cao Xuchuan,Suo Chao,Cui Jing,Duan Xiaochuan,Guo Shaohui,Zhang Xian-Ming
Utilizing plasmonic non-noble metal nanoparticles (NPs) for photocatalytic hydrogen evolution reaction is a significant step toward green energy production. However, optimizing the interface between non-noble metal NPs and semiconducting materials in metal-semiconductor composites remains challenging owing to the inevitable surface oxide layers of non-noble metal NPs because the surface oxide layers of non-noble metal NPs can suppress the transfer of photoinduced carriers, leading to poor photocatalytic performance. Herein, we propose a photoinduced interface activation strategy to reduce the number of oxide layers based on a dynamic charge-transfer mechanism under illumination conditions, with Bi NPs and a Ni-based metal-organic framework (MOF) selected as model materials. Under light illumination, the photoinduced charges and plasmonic hot electrons heavily pooled at the interface between the Bi NPs and Ni-MOF, resulting in the reduction of the oxide layer on the surface of Bi, thus attenuating its hindering effect on charge transfer. This phenomenon led to a dynamically enhanced carrier concentration in the Bi/Ni-MOF composite, with an outstanding photocatalytic hydrogen evolution rate of 5822 µmol g −1 h −1 achieved with the composite. The results of this study indicate that our strategy provides a new method for optimizing plasmonic non-noble metal Bi NPs with oxide layers.
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FUEL
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2025
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IF 7.5
Han Yang,Jing Li,Qiang Chang,Qun-chao Zhao,Meng-na Zhang,Huan-jiang Wang,Cheng-hua Zhang,Fei Wang,Xiao-dong Wen
The catalytic production of hydrogen (H 2 ) through the decomposition of ammonia (NH 3 ) using non-noble metal catalysts with small nanoparticles and high electronegativity at elevated loadings is considered a promising approach for efficient on-site H 2 production. However, excessive loading may undermine the interactions between the metal and the support, resulting in sintering and deactivation of the active components in catalysts at high temperatures. Herein, a layered nickel (Ni) phyllosilicate with varying Ni content was successfully synthesized using amorphous silicon nitride (Si 3 N 4 ) as the silica source through a straightforward deposition–precipitation method. The characterization of Si 3 N 4 -derived Ni phyllosilicate indicates that it is more thermally stable than fumed SiO 2 -derived Ni phyllosilicate when used as a catalyst precursor. Upon 700 °C reduction of Si 3 N 4 -derived Ni phyllosilicate containing 20.0 wt% Ni, small-sized (4.2 nm) and highly dispersion Ni nanoparticles were formed and embedded within the unreduced Ni Phyllosilicate matrix (NiPS-Red700). More importantly, the NiPS-Red700 is presented for efficient catalytic activity and stability for NH 3 decomposition at 700 °C with a gas hourly space velocity (GHSV) of 60,000 mL/g cat /h, being much superior to Ni/SiO 2 catalysts prepared from the same synthesis method. The exceptional catalytic performance of NiPS-Red700 arises from the synergy of highly dispersed and electron-rich Ni nanoparticles, which facilitate the dissociation of the N–H bond and promote the combination of surface N* for N 2 associative desorption, ultimately enhancing the decomposition of NH 3 .
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Changzhou Chen,Xialin Ji,Yongzhi Xiong,Jianchun Jiang
Exploring an advanced catalytic strategy for the high value utilization of lignin derived chemicals into value-added aromatics has attracted tremendous sights for green manufacturing. In this paper, a series of bifunctional 3D rod-shaped mesoporous NiCe metal–organic framework catalysts coupling with hydrogen-donner solvent were reported for the hydrodeoxygenation of vanillin to obtain 2-methoxy-4-methylphenol. Under the optimal conditions, 3Ni-Ce/C catalyst realized the highest conversion of vanillin (>95.0 %) and selectivity of 81.4 % in the absence of additional hydrogen pressure. The characterization results indicated that the interaction of metallic Ni and CeO 2 promoted the generation of Ni-CeO 2-x interface and oxygen vacancies (Ov), which could efficiently adsorb and activate aldehyde group of vanillin to obtain reactive intermediates. And then metallic Ni sites activated the hydrogen-donner solvent to form adsorbed H atoms, which then spilled over to the adjacent Ov to stabilized reactive intermediates. Whereafter, bifunctional 3D rod-shaped mesoporous NiCe metal–organic framework catalysts achieved the hydrodeoxygenation upgrading of vanillin to obtain 2-methoxy-4-methylphenol. Density functional theory (DFT) calculations further revealed that the synergistic effect of Ni-CeO 2 and oxygen vacancies promoted the activation and dissociation of aldehyde group bond in vanillin, enhanced the ability of protonation hydrogenolysis. Additionally, 3Ni-Ce/C catalyst displayed robust activity for no less than four recycles, which provided a feasible method for the build of simultaneous utilization of lignin derivates to value-added fuels and chemicals.
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INDUSTRIAL CROPS AND PRODUCTS
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2024
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IF 5.6
Xialin Ji,Xiaoke Tian,Mengqing Zhou,Changzhou Chen,Jianchun Jiang
In this study, different kinds of lignin, including enzymatic hydrolysis of lignin (EHL), alkaline lignin (AL), kraft lignin (KL) and sodium lignosulfonate (LS) were investigated as precursor to prepare Ni@BTC@X (X= EHL, AL, KL, LS) catalysts using a traditional hydrothermal method with Ni-MOF for HDO upgrading of lignin derivative vanillin (VAN) to generate high value chemical 2-methoxy-4-methylphenol (MMP). The catalytic performance of these catalysts was investigated under different reaction conditions, and it was explored that the conversion of VAN was close to 100 % and the MMP yield was close to 90 % under the optimal conditions (Ni@BTC@LS catalyst, 220 ℃, 4 h, isopropanol, 2 MPa N 2 ). Various physical-chemical characterization results verified that the effects of active sites Ni, porous structure of lignin biochar support and electronic properties of the catalysts played a significiant role in HDO of lignin derived VAN. Additionally, synergistic effect of the highly homogeneously dispersed oxygen vacancies and acidic sites also promoted the VAN conversion efficiency. This work developed a strategy combing the advantages of MOFs and biomass derived substrates for manufacturing novel lignin/MOFs materials in the catalytic field.
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CHEMOSPHERE
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2024
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IF 8.1
Bingnan Zhou,Bo Fan,Zhimin Gong,Shuai Shao,Dongmei Zhou,Shixiang Gao
The excessive usage and emissions of triclosan (TCS) pose a serious threat to aquatic environments. Iron-based bimetallic particles (Pd/Fe, Ni/Fe, and Cu/Fe, etc.) were widely used for the degradation of chlorophenol pollutants. This study proposed a novel synthesis method for the preparation of Ni/Fe bimetallic particles (Ni-Fe bm ) by ball milling microscale zero valent iron ZVI (mZVI) and NiSO 4 . Ball-milling conditions such as ball-milling time, ball-milling speed and ball-to-powder ratio were optimized to prepare high activity Ni-Fe bm bimetallic particles. During the ball-milling process, Ni 2+ was reduced to Ni 0 and formed a coupled structure with ZVI. The amount of Ni 0 on ZVI significantly affected the activity of Ni-Fe bm bimetallic particles. The highest activity Ni-Fe bm bimetallic particles with Ni/Fe ratio of 0.03 were synthesized under optimized conditions, which could remove 86.56% of TCS (10 μM) in aerobic aqueous solution within 60 min. In addition, higher particle dosage, lower pH condition and higher reaction temperature were more conducive for TCS degradation. The higher corrosion current and lower electron transfer impedance of Ni-Fe bm bimetallic particles were the main reasons for its high activity. The hydrogen atom (•H) on the surface of Ni-Fe bm bimetallic particles was mainly contributed to the removal of TCS, as reductive transformation products of TCS were detected by LC-TOF-MS. Notably, a small amount of oxidation products were discovered. The total dechlorination rate of TCS was calculated to be 39.67%. After eight reaction cycles, the residual Ni-Fe bm bimetallic particles could still degrade 28.34% of TCS within 6 h. Low Ni 2+ leaching during reaction indicated that Ni-Fe bm bimetallic particles did not pose potential environmental risks. The prepared environmental-friendly Ni-Fe bm bimetallic particles with high activity have great potential in the degradation of other chlorinated organic compounds in wastewater.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Xiaocui Lai,Wenkai Cao,Ganggang Zhang,Edison Huixiang Ang,Liu Su,Cong Liu,Weihua He,Weihua Lai,Shengliang Deng
The presence of multiple pesticide residues in fruits and vegetables poses a serious threat to human health. Conventional gold nanoparticles (AuNPs) used in multiplex lateral flow immunoassays (M−LFIA) often exhibit poor sensitivity and potential for misidentification. This study introduces a traffic signal-inspired fluorescent LFIA (T-FLFIA) designed for the simultaneous quantitative detection of chlorothalonil (CTN), paclobutrazol (PBZ), and fipronil (FIP) in cowpea and apple samples. Utilizing the hydrophobic interactions of aggregation-induced emission luminogens (AIEgens) and the coordination of epicatechin (EC) with Ni 2+ , we developed a novel nanostructure-aggregation-induced emission nanoparticle (AIENP) coated with a metal-polyphenol network of Ni/EC (AIENP@Ni/EC) via a self-assembly method and employed it as fluorescence probe in T-FLFIA. Three distinct colors of AIENP@Ni/EC featuring green, yellow, and red fluorescence were successfully synthesized by coating various AIEgens. This multicolor fluorescence capability facilitates more precise and expedited discrimination among multiple detection targets. High-performance AIE fluorescence probes were fabricated by directly coupling AIENP@Ni/EC with different antibodies through electrostatic interactions, leveraging the exceptional biocompatibility of Ni/EC. The T-FLFIA exhibited sensitive detection of CTN, PBZ, and FIP at concentrations as low as 0.038 ng/mL, 0.025 ng/mL, and 0.046 ng/mL, respectively, with high qualitative accuracy (92.5 %) within a rapid timeframe (5 s). This exceptional performance can be attributed to its outstanding optical properties and distinguishable colors. This approach demonstrated enhanced sensitivity and accuracy, reduced consumption of antibodies and immunoprobes, and a broader detection range compared to single-color AuNPs-M−LFIA. This study introduces a novel, practical, and cost-effective tool for rapid screening of diverse pesticide residues in field settings.
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