JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL
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2016
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IF 3.958
Huan Chen,Ting Li,Fang Jiang,Zhe Wang
Catalytic reduction of N -nitrosodimethylamine (NDMA) was investigated over γ-Al 2 O 3 supported bimetallic Pd-Ni catalysts (3%(Pd x Ni 1−x )). NDMA could be reduced to dimethylamine over 3%(Pd 0.8 Ni 0.2 ) with a metal-loading-normalized pseudo-first-order rate constant of 836 ± 21 L g me −1 h −1 . Characterization results showed that the reducibility of PdO (or NiO) was improved by addition of Ni (or Pd) in 3%(Pd x Ni 1−x ); Pd-Ni ensembles were formed in 3%(Pd x Ni 1−x ) and there was an electronic transfer from Pd to Ni; metal dispersion was affected by the formation of Pd-Ni ensembles and a volcano curve of metal dispersion via Pd/Ni ratio was observed. The activity profiles demonstrated that TOF had a significant positive relationship with metal dispersion of 3%(Pd x Ni 1−x ), indicating high metal dispersion favor NDMA reduction. NDMA reduction over 3%(Pd 0.8 Ni 0.2 ) catalyst could be described by Langmuir-Hinshelwood model, reflecting an adsorption controlled reduction mechanism. The reduction mechanism of NDMA over 3%(Pd 0.8 Ni 0.2 ) catalyst was proposed to be that H 2 was activated by Pd, and H spillover from Pd to Ni/NiO reduced NDMA though N-N cleavage.
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JOURNAL OF APPLIED ELECTROCHEMISTRY
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2016
·Vol. 46
·期 12
·1177-1186
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IF 2.223
Guo Jie,Hou Yongjiang,Li Bo,Wang Yaquan
Abstract The Ni–B-modified carbon paste electrodes were synthesized by the electroless deposition, followed by thermal treatment. Scanning electron microscopy, X-ray diffraction, and X-ray photoelectron spectroscopy were performed to gather information about the morphology, crystallinity, and binding energy. The fabricated Ni–B/C electrodes are applied to methanol electrooxidation in alkaline media. The results show that Ni–B/C catalyst with a comparable amount of microcrystalline Ni and Ni 3 B, 59 and 41 wt%, displayed a significantly enhanced electrocatalytic activity, which is approximately three times the activity of the unheated Ni–B/C catalyst. The synergetic mechanism of methanol oxidation was proposed that involves one Ni 3 B site favor the adsorption and activation of the methanol molecule and one Ni site for oxidative mediation of methanol. In addition, the kinetic parameters of the reaction were calculated using linear sweep voltammetry. Graphical abstract The illustration of the speculated methanol oxidation mechanism.
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DALTON TRANSACTIONS
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2024
·Vol. 53
·期 23
·9724-9731
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IF 3.5
Ying Peng,Shuo Chen,Zhengli Hu,Mengqi Yin,Lishun Pei,Qiaohua Wei,Zailai Xie
Developing novel electrocatalysts for achieving high selectivity and faradaic efficiency in the carbon dioxide reduction reaction (CO2RR) poses a major challenge. In this study, a catalyst featuring a nitrogen-doped carbon shell-coated Ni nanoparticle structure is designed for efficient carbon dioxide (CO2) electroreduction to carbon monoxide (CO). The optimal Ni@NC-1000 catalyst exhibits remarkable CO faradaic efficiency (FECO) values exceeding 90% across a broad potential range of −0.55 to −0.9 V (vs. RHE), and attains the maximum FECO of 95.6% at −0.75 V (vs. RHE) in 0.5 M NaHCO3. This catalyst exhibits sustained carbon dioxide electroreduction activity with negligible decay after continuous electrolysis for 20 h. More encouragingly, a substantial current density of 200.3 mA cm−2 is achieved in a flow cell at −0.9 V (vs. RHE), reaching an industrial-level current density. In situ Fourier transform infrared spectroscopy and theoretical calculations demonstrate that its excellent catalytic performance is attributed to highly active pyrrolic nitrogen sites, promoting CO2 activation and significantly reducing the energy barrier for generating *COOH. To a considerable extent, this work presents an effective strategy for developing high-efficiency catalysts for electrochemical CO2 reduction across a wide potential window.
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PubMed
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-15
·
IF 14.7
Yao Zhibo,Cheng Hao,Xu Yifei,Zhan Xinyu,Hong Song,Tan Xinyi,Wu Tai-Sing,Xiong Pei,Soo Yun-Liang,Li Molly Meng-Jung,Hao Leiduan,Xu Liang,Robertson Alex W.,Xu Bingjun,Yang Ming,Sun Zhenyu
The electrocatalytic reduction of CO 2 to CO is slowed by the energy cost of the hydrogenation step that yields adsorbed *COOH intermediate. Here, we report a hydrogen radical (H•)-transfer mechanism that aids this hydrogenation step, enabled by constructing Ni-partnered hetero-diatomic pairs, and thereby greatly enhancing CO 2 -to-CO conversion kinetics. The partner metal to the Ni (denoted as M) catalyzes the Volmer step of the water/proton reduction to generate adsorbed *H, turning to H•, which reduces CO 2 to carboxyl radicals (•COOH). The Ni partner then subsequently adsorbs the •COOH in an exothermic reaction, negating the usual high energy-penalty for the electrochemical hydrogenation of CO 2 . Tuning the H adsorption strength of the M site (with Cd, Pt, or Pd) allows for the optimization of H• formation, culminating in a markedly improved CO 2 reduction rate toward CO production, offering 97.1% faradaic efficiency (FE) in aqueous electrolyte and up to 100.0% FE in an ionic liquid solution.
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ACS Applied Nano Materials
·
2024
·
IF 5.3
Xi-ya Shan,Xing-hai Zhou,Wen-qi Cui,Min-yu Li,Yuan-lin Yan,Yong-fang Qian,Yuan Gao,Shang-ru Zhai,Li-hua Lyu,Hong-zhu Liu,Zhong-gang Wang
Ingenious microstructure design and suitable component regulation are the prevailing methods to meet the requirements of lightweight, broadband, and high-efficiency electromagnetic absorbing materials. Herein, petal-like magnetic Ni nanosheets on porous carbon nanofibers (Ni-PCF) are synthesized by electro-blown spinning, hydrothermal reaction, and high-temperature calcination. The construction of a porous carbon fiber skeleton originated from the in situ composition of the pore-forming agent (polystyrene (PS)), and the formation of petal-like magnetic Ni nanosheets was derived from self-assembling during a hydrothermal reaction. The porous carbon fiber skeleton and petal-like Ni nanosheets could not only generate multiple reflections to extend the transmission pathway but also induce a synergistic effect of magnetic loss and dielectric loss to promote impedance matching, giving rise to more electromagnetic wave attenuation and energy dissipation. The good impedance matching, multiple reflections, and synergetic electric/magnetic losses originating from ingenious microstructures and suitable multicomponents resulted in the best microwave absorption performance of Ni-PCF2 with a minimum reflection loss (RLmin) value of 37.93 dB at 6.08 GHz and an effective absorption bandwidth (EAB) of 4.43 GHz.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Shujie Liang,Jiaxin Lv,Yishun Wang,Hong Deng
The development of efficient and stable single-atom catalysts (SACs) for CO 2 photoreduction is a persistent challenge. This study reports the successful preparation of SACs by incorporating isolated Ni atoms into carbon nanorods through a low-temperature calcination process using nickel bis(dimethylglyoximate) complexes. These Ni atoms, maintaining their original coordination environments, can facilitate charge separation, and enhance CO 2 adsorption and activation. The optimized catalyst exhibits a CO formation yield of 24.4 µmol with ∼96 % selectivity in high-purity CO 2 , outperforming both the precursor and pure carbon. Additionally, the Ni SACs showed strong catalytic selectivity in diluted CO 2 conditions, with selectivity rates of 82.57 %, 80.35 %, and 61 % at 0.1, 0.05, and 0.01 atm, respectively. This work provides critical insights for designing efficient visible light-responsive CO 2 photoreduction catalysts at the atomic level.
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ACS Applied Nano Materials
·
2024
·
IF 5.3
Chengming Long,Sirui Liu,Di Wang,Zhaoqi Lu,Qiulan Zhang,Qiong Gao,Mingyi Zhang,Xinzhi Ma
Photoelectrochemical hydrogen production technology holds promise for directly and swiftly generating green hydrogen, which is pivotal for human welfare; however, it faces challenges posed by the energetically sluggish oxygen evolution reaction (OER). Cobalt-based nitrides are considered excellent photoelectrochemically active in the OER (PEOER) catalysts, and their conductivity and photoconversion efficiency remain relatively low. This paper presents the fabrication of Ni-alloyed Co4N nanowire arrays on carbon cloth ((Co1–xNix)4N NWAs/CC) as PEOER catalysts. By analyzing advanced in situ Raman and X-ray photoelectron spectroscopy (XPS) results, we discovered that Ni not only enhances the conductivity of the catalyst but, more importantly, also creates more photoexcited Co2+ OER centers and favors its reconstruction to CoOOH to charge PEOER. Furthermore, nitrogen plays a critical role in transforming pyridinic nitrogen into other forms of nitrogen to stabilize the catalyst’s structure. These advantages endow (Co0.74Ni0.26)4N NWAs/CC with remarkable PEOER enhancement (988%), which drives the standard current density of 10 mA cm–2 with only a 283 mV overpotential along with good durability. This research provides insights into the PEOER mechanisms of cobalt-based transition metal nitrides, providing a way for designing next-generation PEOER catalysts.
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Materials Chemistry Frontiers
·
2024
·
IF 6
Mohit Kumar,Bhimanaboina Ramulu,Jae Su Yu
To produce clean and green hydrogen energy from electrolytic water, better electrocatalytic materials need to be developed. Herein, we reported the development of a Ti3C2 MXene@Ni/Co sulfide hybrid material for the use in hydrogen evolution reaction (HER) process, which is effective and stable. The shape of metal sulfide and its interactions with Ti3C2 MXene caused electronic coupling. This increased both the exposed metal sulfide's active edge sites and the charge-transfer speed. When compared with pure MXene and Ti3C2 MXene@NiS nanostructure, Ti3C2 MXene@Co4S3 exhibited outstanding electrocatalytic activity and stability in the HER process. The unique properties of the skeletal structure and the robust interface interaction between Co4S3 and MXene are responsible for the superior performance of Ti3C2 MXene@Co4S3 in the HER process. Our research offers a practical method to synthesize specialized nanostructures for electrocatalysis, electronics, and other applications.
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ENERGY
·
2018
·
IF 4.968
Lin Li,Dawei Tang,Yongchen Song,Bo Jiang,Qian Zhang
In this work, a ceria promoted Ni-based catalyst supported in mesoporous montmorillonite (MMT) was developed and evaluated in ethanol steam reforming . This Ni-Ce/MMT catalyst was synthesized by an ultrasound assisted cation exchange impregnation method and characterized by X-ray diffraction, N 2 adsorption–desorption, H 2 temperature-programmed reduction and transmission electron microscopy. TEM images of Ni-Ce/MMT presented that narrow Ni nanoparticles (av. 6.0 nm) were uniformly deposited within the mesoporous MMT support. This was attributed to the strong interaction between Ni and ceria and the confinement effect from the framework of MMT support. The catalytic activity and stability of Ni-Ce/MMT were studied in steam ethanol reforming and compared with Ni/MMT. The higher ethanol conversion and H 2 selectivity of Ni-Ce/MMT demonstrated the addition of ceria facilities the reaction of ethanol steam reforming. Additionally, the ethanol conversion was much more stable on Ni-Ce/MMT than on Ni/MMT during a long-term ethanol steam reforming reaction, illustrating that the catalyst deactivation was preferably suppressed with the help of ceria. In short, the Ni-Ce/MMT is a promising catalyst for ethanol steam reforming owing to the remarkable effect of ceria as well as the confinement effect of MMT support which can effectively suppress the Ni sintering and carbon deposition .
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2017
·
IF 2.843
Hai-Bo Zhao,Zhi-Bing Fu,Xue-Yi Liu,Xiao-Cao Zhou,Hong-Bing Chen,Ming-Long Zhong,Chao-Yang Wang
Novel magnetic and conductive Ni/carbon aerogels have been successfully fabricated through an autocatalytic reduction process. The resultant Ni/carbon aerogels have nanoporous structure with high specific surface area, low densities, appropriate electrical conductivities and controllable magnetization. Due to these special attributes, the aerogel composites are demonstrated to be a great microwave absorbent possessing strong and controllable EM absorption with ultrathin thickness. Only with filler loading of 10 wt % in the wax, a minimum RL of −57 dB is found at 13.3 GHz with the thickness of 2 mm. Even with the thickness of 1.5 mm, the Ni/carbon aerogel-3 composite can exhibit the low RLmin value of −32 dB and wide effective EM absorption bandwidth of 4.0 dB. The synergistic effect of the medium dielectric loss, weak magnetic loss and good impedance match, accounts for the high microwave absorption performance.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2024
·
IF 5.8
Guangcai Ma,Wenbin Li,Fei Wang,Lunyong Zhang,Bin Chen,Xiujun Yu,Wenqing Hu,Ting Ding,Baiyang Zhou,Zhuo Zhang
As an intriguing strategy for massive hydrogen production, photoelectrochemical (PEC) seawater splitting compels the anode to be highly hypochlorite-resistant. Inspired by algae, we designed a robust photoelectrocatalyst that WO 3 nanorods (NRs) are covered by N/W co-doped (Co, Ni, W)O x N y nanosheets (NSs). The NSs expose (111) faces and are decorated by (Co, Ni)WO 4 nanoparticles. DFT calculations reveal that Co and Ni atoms on the (111) surface of N/W co-doped NSs are more likely to adsorb OH - , while W atoms are more favorable to adsorb Cl - . Secondly, the lattice distortion and multi-crystal phases of NSs are triggered by doped W atoms, and the evacuation of 5d electrons makes W atoms as donor centers, leading to enhanced catalytic activity of CoNi atoms and corrosion resistance to Cl - . Furthermore, the N atoms expand the valence band of CoNiO x and elevate the conduction band of (Co, Ni)WO 4 , facilitating more electrons to participate in PEC reaction and the realization of seawater full-splitting. Resultantly, the N/W co-doped (Co, Ni, W)O x N y /WO 3 hetero-NRs (HNRs) demonstrate a PEC current density about 0.35 mA/cm 2 at 1.23 V RHE with durability over 100 hours in seawater. This work provides a practical strategy towards the durable PEC anode for seawater splitting.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Zengjian Cai,Yi Cai,Zhe Wang,Shoujie Liu,Xinhu Liang,Hao Ren,Yanan Cao,Zikang Su,Fengyi Shen,Shitu Yang,Guodong Sun,Xiaoxin Yang,Xueqiang Zhang,Mingzhen Hu,Xingwu Liu,Kebin Zhou
Selective conversion of CH 4 and CO 2 to syngas via the dry reforming reaction is highly desirable in terms of restraining the greenhouse effect and meanwhile acquiring useful chemicals. However, the most promising Ni catalysts for the reaction still suffer from severe coking and thus poor durability. Here, we report that using amorphous Ni nanoparticles synthesized on an N modified mesoporous silica support, the catalytic activity and coke-resistant performance of Ni toward the photothermal dry reforming of methane (DRM) are greatly improved. Theoretical calculations further unveil that the amorphous Ni nanoparticles are much more energetically favorable to activate the CH 4 and CO 2 molecules as well as to remove the C* intermediates for coke formation than their crystalline Ni counterparts, which renders the amorphous Ni nanoparticles with both superb activity and excellent coke-resisting property. This finding possibly provides a new avenue to make both highly efficient and anti-coking catalysts for the DRM reaction and beyond via facile amorphization of active metals.
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