INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
Qikai Ren,Shuaishuai Wang,Haoyu Liu,Xing Zhang,Yanran Cui,Gui-Rong Zhang,Lei Nie,Donghai Mei
The dry reforming of methane (DRM) serves as a pivotal reaction for hydrogen generation and the simultaneous conversion of methane and carbon dioxide, two major greenhouse gases, into syngas that can further be converted into high-value fuels and chemicals. However, catalyst deactivation imposes a major challenge that prohibits the market penetration of DRM. Here we reported a series of bifunctional Ni-Ce catalysts supported on SSZ-13 (Ni-Ce-SSZ-13) and discovered that a small amount of Ce could significantly enhance the activity, selectivity, and stability for DRM. Optimal ratio of Ni to Ce has been identified to yield peak catalytic performance. The optimal performance is correlated with the maximum Ce 3+ /Ce 4+ ratio as revealed by XPS analysis, which implies an increased presence of oxygen vacancies in the catalysts. It played a crucial role in facilitating the oxidation of activated CH 4 species at Ni sites, thereby enhancing DRM activity and diminishing the detrimental coke formation. It is also disclosed that integrating proper amount of Ce fosters its interactions with Ni, effectively preventing the agglomeration of Ni sites. This work presents great implications for the rational design and catalytic synergy of bi-/multi-functional zeolite catalysts for other technological applications.
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Materials
·
2025
·Vol. 18
·期 14
·3419
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IF 3.2
Muhammad Sabir,Mahmoud Sayed,Iram Riaz,Guogen Qiu,Muhammad Tahir,Khuloud A. Alibrahim,Wang Wang
The rapid recombination of photoinduced charge carriers in semiconductors remains a significant challenge for their practical application in photocatalysis. This study presents the design of a step-scheme (S-scheme) heterojunction composed of carbon nitride (g-C3N4) and nickel-based metal–organic framework (Ni-MOF) to achieve enhanced charge separation. The establishment of an S-scheme charge transfer configuration at the interface of the Ni-MOF/g-C3N4heterostructure plays a pivotal role in enabling efficient charge carrier separation, and hence, high CO2photoreduction efficiency with a CO evolution rate of 1014.6 µmol g−1h−1and selectivity of 95% under simulated solar illumination. CO evolution represents an approximately 3.7-fold enhancement compared to pristine Ni-MOF. Density functional theory (DFT) calculations, supported by in situ irradiated X-ray photoelectron spectroscopy (XPS) and electron paramagnetic resonance (EPR) experimental results, confirmed the establishment of a well-defined and strongly bonded interface, which improves the charge transfer and separation following the S-scheme mechanism. This study sheds light on MOF-based S-scheme heterojunctions as fruitful and selective alternatives for practical CO2photoreduction.
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CERAMICS INTERNATIONAL
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2024
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IF 5.1
Jingyu Song,Yongqian Shen,Guibin Zhang,Mingxuan Sun,Mengyao Han,Xueyan Du
While two-dimensional lamellar materials, specifically Ti 3 C 2 T x MXenes, have shown great promise as wave-absorbing materials, the precise design of interlayer spacing poses a persistent challenge. In this study, Ti 3 C 2 T x MXene layers with adjustable interlayer spacings were crafted using a straightforward molecular welding technique. Through the incorporation of Ni nanoparticles onto the Ti 3 C 2 T x MXene layers using a combination of simple mechanical stirring and carbonation reactions, we successfully developed Ti 3 C 2 T x MXene/Ni/C composites featuring a distinct lamellar structure. A uniform dispersion of Ni nanoparticles on the surface of the Ti 3 C 2 T x MXene nanosheets was found with some of the nanoparticles intercalated into the layers. The Ti 3 C 2 T x MXene/Ni/C composites exhibited a maximum reflection loss (RL) value of −42.3 dB at 12.3 GHz, accompanied by an impressive effective absorption bandwidth (EAB) of 5.6 GHz. This outstanding absorption performance could be attributed to various factors, including the dielectric loss of the Ti 3 C 2 T x MXene lamellae, reflections and scattering of multiphase heterostructures, the magnetic loss of the Ni nanoparticles, and their synergistic attenuation. Furthermore, Ni nanoparticles with high electrical conductivity induced vortex currents under the alternating influence of electromagnetic waves (EMWs), resulting in a substantial depletion. This study introduces an innovative approach for synthesizing Ti 3 C 2 T x MXene/Ni/C composites with tunable interlayer spacing, showing their potential for applications in microwave absorption (MA).
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CHEMICAL ENGINEERING JOURNAL
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2025
·
IF 13.2
Jianlong Wang,Honglin Yan,Cheng Wei,Yuan Ha,Weidong Zhu,Lu Li,Chaoyi Zhou,Qianxin Xiang,Zhimin Li,Yue Hao
Ultra-high Ni layered cathodes LiNi x Mn 1- x O 2 ( x > 0.9) with high energy density for lithium-ion batteries suffer from severe fatigue failure upon cycling because of the unstable crystal structures at highly delithiated states. Despite efforts to address this issue, enhancing the structural stability by electrostatic interaction between oxygen layers has been overlooked. Herein, we propose an electrostatic interaction strategy via Mn-Mg-Al-Ti medium-entropy doping to improve the fatigue resistance of the crystal structure. As expected, these chosen dopants efficiently impede the distortion, interlacement, and fracture of transition metal slabs in crystal structures by enhancing the electrostatic interaction. Accordingly, the cathode LiNi 0.93 Mn 0.04 Mg 0.01 Al 0.01 Ti 0.01 O 2 delivers superior cycling performance with a capacity retention of 96.1 % at 0.5C after 100 cycles. This work demonstrates the effectiveness of improving the electrochemical performance of ultra-high Ni cathodes by the electrostatic interaction strategy, which is of great significance for their commercial application.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-12
·
IF 15.7
Zhao Xin,Li Changzhi,Wen Jie,Qiang Qian,Shen Zirong,Yu Haipeng,Zhou Xin,Yue Fengxia,Fang Ruiqi,Li Yingwei,Zhang Tao
Lignin refining still suffers from great challenges of selective depolymerization and cleavage of stubborn C‒C linkages. Here, a robust atomically dispersed Cu/Ni-SA@HNC catalyst is fabricated for super-selective hydrogenolysis of lignin and model compounds via an unusual “preferential C α –C β bond cleavage in β-O-4 linkages” pathway, affording toluene in yield up to 75.7% from β-O-4 model compounds, and up to 33.7 ± 1.6 wt% (nine parallel experiments) from poplar lignin. The catalyst exhibits high stability, and the scale-up potential is demonstrated by the high space-time yield of toluene (33.7 g·g cat −1 ·h −1 ) in continuous flow reaction of β-O-4 model compound. The origin of the extraordinary selectivity towards C α –C β bond cleavage rather than C‒O bond cleavage in β-O-4 model compounds is uncovered. This work conquers the major challenges in lignin valorization by using non-noble dual-metal single-atom catalyst, not only showcasing the application perspective of atomically dispersed catalysts in biopolymer refinery, but also providing a cost-efficient, petroleum independent solution to valuable commodity chemicals.
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AICHE JOURNAL
·
2025
·
IF 4
Hong-Da Zhang,Wei-Yao Yang,Miao Pang,Ya-Qiao Tian,Shi-Chao Su,Zhi-Ping Zhao,Le Sang
Non-modified Pd/PDA/Ni foam, hydrophobic modified F 9 -Pd/PDA/Ni foam, and F 17 -Pd/PDA/Ni foam catalysts are successfully prepared and used for NB hydrogenation in micropacked bed reactors (μPBRs). The catalytic performance increases with the addition of water in the water–methanol mixed solvent. In the mixed solvent with 50 v/v% water, F 17 -Pd/PDA/Ni foam can almost completely convert nitrobenzene (NB) with a yield of 95.9% at a mild 45°C. As the solvent contact angle of catalysts increases (87.5–141.5°), the enhancement ratios of NB conversion and AN yield are 28.9%–92.4% and 31.4%–106.5%, respectively. The space–time yield of AN in μPBRs reaches 1.873 kg·L −1 ·h −1 ·g −1 , which is 1–2 orders of magnitude higher than that of conventional reactors. The kinetic model of NB hydrogenation is established at the water–methanol system in μPBRs. The hydrophobicity of catalysts significantly improves the reaction rate of NB hydrogenation, and the reaction rate constant is increased by 69.9%.
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LANGMUIR
·
2025
·
IF 3.9
Xuan Chen,Zheng Chen,Lang Wu,Feifei Hu,Xin Zhou,Qian Lin,Hongyan Pan,Yongyong Shi,Donghai Jiang
Using an l-arginine (LA)-functionalized Pd–Ni catalyst, hydrogen peroxide (H2O2) was directly synthesized via a self-designed microreactor at ambient temperature and pressure. The yield of H2O2 achieved 574.31g kgcat–1 h–1, with the concentration of H2O2 in the solution reaching 4.05 wt % per hour. After five cycles and online activation, the LA functionalized Pd–Ni catalyst maintained high H2O2 catalytic activity. The catalytic activity evaluation experiments, characterization results, and simulation studies demonstrated that Ni doping and LA-functionalization synergistically modulate the electronic structure of the active Pd component. This modulation increases the concentration of Pd2+ at the active sites, effectively inhibits the dissociation of the O–O bond in O2*, OOH*, and HOOH* species, thereby enhancing the catalytic performance for H2O2 production. This study proposes a systematic strategy for the design of Pd-based catalysts to directly synthesize highly efficient H2O2.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Guolin Zhang,Qi Xu,Hui Huang,Fei Zhou,Liangyun Yu,Qi Chen,Jiarong Yang,Yanli Xiao,Qi Zhang
The extensive use of fossil fuels has resulted in large amounts of carbon dioxide being emitted into the air and has led to a number of environmental problems. Given the abundance of both carbon dioxide and sunlight in the earth’s atmosphere, converting solar energy into chemical energy by photothermally catalyzing carbon dioxide hydrogenation to produce methanol is a potential strategy. By using the coprecipitation approach, a Ni-doped In2O3 catalyst was created, and its compositional valence, morphology, specific surface area, band gap, and other properties were assessed by XRD, XPS, TEM, BET, H2-TPR, CO2-TPD, and UV–vis characterization. Methanol production from carbon dioxide hydrogenation is stable and effective under lower pressure (1 MPa) photothermal settings, with an efficiency of 63.4 gMeOHh–1kgcat–1, which is approximately 120% higher than that of pure In2O3 under the same circumstances.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Bowen Lu,Ziqiang Han,Xinyu Zhi,Liqi Zhang
NiFe 2 O 4 exhibits excellent redox properties and is widely applied in catalytic reactions. However, rapid inactivation under reaction conditions limited its industrial applications. In this study, CeO 2 -NiFe 2 O 4 composite catalysts were synthesized, and the Reverse Water Gas Shift (RWGS) reaction was measured to reveal its CO 2 hydrogenation performance under a high-temperature condition. NiFe 2 O 4 catalysts got deactivated after being reduced to Fe-Ni alloy at 700 °C, decreasing the CO 2 conversion rate. CeO 2 addition can significantly improve its high-temperature activity, and 20CeO 2 -NiFe 2 O 4 exhibited the best catalytic activity (80.85 %, 700 °C). The CeO 2 -confined maintained Ni-Fe alloy with a relatively small crystal size and larger specific surface area, supporting more active sites for CO 2 hydrogenation. CeO 2 addition induced higher oxygen vacancy concentration, enhancing CO 2 activation and formates species formed on 20CeO 2 -NiFe 2 O 4 , resulting in higher CO 2 conversion activity. In addition, 20CeO 2 -NiFe 2 O 4 maintained its catalytic stability for 50 h at 700 °C. The CeO 2 confined enhanced the high-temperature stability of Fe-Ni alloy. CeO 2 and formed CeFeO 3 dispersed in 20CeO 2 -NiFe 2 O 4 inhibited excessive aggregation of Fe-Ni alloy, and CeO 2 inhibited carbon deposition on Fe-Ni alloy, improving Fe-Ni alloy’s reaction stability under RWGS reaction conditions. CeO 2 confined may give insight into improving metal stability under high-temperature and reductive conditions in heterogeneous catalysis.
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ACS Catalysis
·
2021
·
IF 13.084
Huiyuan Cheng,Xuemei Wu,Manman Feng,Xiangcun Li,Guangping Lei,Zihao Fan,Dongwei Pan,Fujun Cui,Gaohong He
Developing diatomic catalysts (DACs) for the CO2 reduction reaction (CO2RR) has emerged as a promising leading-edge research area owing to their maximum atomic utility and more sophisticated functionalities. However, the proper design of DACs at an atomic level and an understanding of the synergistic mechanism of binary sites remain challenging. Herein, an N-rich carbon matrix with precisely controlled Ni/Cu dual sites is synthesized through the assistance of metal–organic frameworks. The as-prepared catalyst presents high CO Faradaic efficiency of over 95% from −0.39 to −1.09 V vs reversible hydrogen electrode (RHE) with the maximum value of 99.2% at −0.79 V vs RHE and long-term durability of 60 h electrolysis. Density functional theory studies reveal that the electronic redistribution and band gap narrowing induced by the adjacent NiN4 and CuN4 moieties enhance the electron conductivity and strengthen the bonding interactions between *COOH intermediates and Ni centers, thus lowering the overall reaction barriers and promoting CO generation.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Xia Wei,Tianyao Wang,Hongbin Dai,Song Li
The hydrazine oxidation reaction (HzOR) plays a critical role in direct hydrazine fuel cells and presents a promising alternative to the kinetics-sluggish oxygen evolution reaction in water reduction. Engineering catalysts with high-density multifold nanotwin structures has emerged as a compelling strategy to enhance catalytic activity. However, the exploration of multifold nanotwins for HzOR applications remains absent. Herein, we report the successful synthesis of a porous Ni-Zn-Cu catalyst featuring high-density twofold and fivefold nanotwins. The Ni-Zn-Cu catalyst supported on Ni foam (Ni-Zn-Cu/Ni foam) exhibits exceptionally high catalytic activity and stability toward the HzOR, achieving a current density of 204.3 mA cm −2 at 0.0 V vs. RHE and retaining up to 89.1 % after 20 h of continuous electrolysis. Online mass spectrometer (MS) analysis indicates that the Ni-Zn-Cu coating facilitates N N bond cleavage of N 2 H 4 . This study offers valuable insights into the development of multifold nanotwin catalysts for advancing HzOR applications.
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Journal of the American Chemical Society
·
2024
·
IF 14.4
Jiyue Zhang,Wenda Wang,Xiaowei Chen,Jinlong Jin,Xiaojun Yan,Jianmei Huang
As an efficient and clean energy carrier, hydrogen is expected to play a key role in future energy systems. However, hydrogen-storage technology must be safe with a high hydrogen-storage density, which is difficult to achieve. MgH2 is a promising solid-state hydrogen-storage material owing to its large hydrogen-storage capacity (7.6 wt %) and excellent reversibility, but its large-scale utilization is restricted by slow hydrogen-desorption kinetics. Although catalysts can improve the hydrogen-storage kinetics of MgH2, they reduce the hydrogen-storage capacity. Single-atom catalysts maximize the atom utilization ratio and the number of interfacial sites to boost the catalytic activity, while easy aggregation at high temperatures limits further application. Herein, we designed a single-atom Ni-loaded TiO2 catalyst with superior thermal stability and catalytic activity. The optimized 15wt%-Ni0.034@TiO2 catalyst reduced the onset dehydrogenation temperature of MgH2 to 200 °C. At 300 °C, the H2 released and absorbed 4.6 wt % within 5 min and 6.53 wt % within 10 s, respectively. The apparent activation energies of MgH2 dehydrogenation and hydrogenation were reduced to 64.35 and 35.17 kJ/mol of H2, respectively. Even after 100 cycles of hydrogenation and dehydrogenation, there was still a capacity retention rate of 97.26%. The superior catalytic effect is attributed to the highly synergistic catalytic activity of single-atom Ni, numerous oxygen vacancies, and multivalent Tix+ in the TiO2 support, in which the single-atom Ni plays the dominant role, accelerating electron transfer between Mg2+ and H– and weakening the Mg–H bonds. This work paves the way for superior hydrogen-storage materials for practical unitization and also extends the application of single-atom catalysis in high-temperature solid-state reactions.
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