AICHE JOURNAL
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2025
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IF 4
Bin Chen,Xingwen Cha,Xuexue Dong,Juanjuan Bian,Jiale Huang,Qingbiao Li,Xiaoqing Huang,Guowu Zhan
Upgrading biomass-derived fatty acids through the H 2 -free and solvent-free catalytic deoxygenation process is both safe and eco-friendly. Herein, we used modified rice husk-derived biochar with ultra-high specific surface area and abundant surface groups as a support to design a homologous bimetallic site catalyst containing Ni single atoms (Ni 1 ) and Ni nanoclusters (Ni n ), the synergy between which is dedicated to excellent catalytic performance. The designed catalyst, Ni 1+n /A-bio-AC, demonstrated an impressive 89.8% selectivity for odd-numbered long-chain alkanes during the H 2 -free and solvent-free deoxygenation of stearic acid, with a turnover frequency value over 18 times higher than conventional Ni/AC. Multiple characterizations revealed the coexistence of Ni 1 and Ni n on the catalyst support. Experimental and theoretical calculations showed that Ni n facilitates the adsorption of fatty acid substrates. While Ni 1 serves as highly dispersed Lewis acid sites, enhancing the dehydrogenation of fatty alcohol intermediates during the in situ hydrodeoxygenation and lowering the decarboxylation pathway energy barriers via electronic synergy with Ni n , thus remarkably boosting the catalytic deoxygenation activity. This work provides a novel Ni dual-site catalyst for developing biomass resource conversion technologies.
研究领域:
催化化学
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生物质能
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
Small
·
2022
·Vol. 18
·期 26
·2201996
·
IF 15.153
Tengfei Zhang,Hong Xiao,Xiao Liang,Fanchao Zhang,Huifeng Zhuang,Qiuming Gao,Lirong Zheng
A universal strategy is established for preparing the carbonaceous matrix-based atomically distributed metal catalysts M-BPC (M=Ni, Co, Fe, Cu, and Mn, and biomass-derived porous carbon (BPC)) by one-step pyrolysis of mixed metal salts and biomass alfalfa. The optimized Ni-BPC has dual-atom Ni(II) 2 N 4 (µ 2 -N) 2 moieties, which are chemically anchored on the alfalfa-derived developed porous N-doped carbon BPC matrix. An ultrahigh specific surface area of 3133 m 2 g −1 with huge total pore volume of 3.02 cm 3 g −1 is obtained for Ni-BPC. The Ni-BPC could greatly promote the redox kinetics and effectively prevent the shuttle effect of lithium polysulfides in a Li–S battery. The Li–S battery assembled with the Ni-BPC modified separator exhibits prominent rate performance with the reversible specific capacities of 1279, 1119, 1037, 948 and 787 mAh g −1 at the current densities of 0.1, 0.2, 0.5, 1 and 2 C, respectively. The battery presents an ultra-long life with low capacity decay of 0.028% per cycle up to 2100 cycles at 1 C. Even under high areal S loadings of 3.9 mg cm −2 , the high discharge capacity of 976.6 mAh g −1 is obtained at 0.2 C and excellent cycling stability with 61.1% capacity retention is achieved after 490 cycles.
研究领域:
材料科学
·
能源存储
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Xingguo Wang,Yingying Qin,Jian Lu,Weidong Qin,Honghui Teng
Graphitic carbon nitride (g-C 3 N 4 , CN) has garnered significant attention in the field of photocatalytic hydrogen production due to its unique electronic structure and ease of functional modification. However, the photocatalytic performance of CN is substantially limited by sluggish charge carrier dynamics and a scarcity of active centers. Herein, a novel photocatalyst is designed by modifying CN with nickel atoms and introducing benzene rings (Ni-BCN) onto its structure. The optimized Ni-BCN photocatalyst demonstrates remarkable photocatalytic activity without Pt as a co-catalyst. The hydrogen evolution rate reaches 1844.3 μmol g -1 h −1 , which is nearly 49.7 times higher than that of pristine CN. This significant enhancement is primarily attributed to the fact that the introduction of benzene rings into the CN framework provides driving force for improving charge separation within the in-plane, optimizing the energy band through an extended π-conjugated structure to enhance light absorption, and forming van der Waals heterojunctions that facilitates interlayer electron flow. Additionally, nickel atoms as active sites accelerate proton adsorption and reduce the free energy barriers of hydrogen evolution. This work purposefully optimizes the properties of CN by regulating its molecular structure, thereby fully leveraging these advantages in photocatalytic hydrogen evolution.
研究领域:
材料科学
·
光催化
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Jun Wan,Yang-Ai Ma,Yina Nie,Junhao Cheng,Chengming Wang,Lin Liu,Feng Fu
Photocatalytic selective aerobic oxidation in organic synthesis is a green and sustainable approach to producing valuable chemicals. However, the sluggish charge dynamics and limited active sites for O 2 activation tremendously hinder catalytic activity. Herein, we address these challenges by developing a novel polarization photocatalyst composed of atomically dispersed Ni sites with S-doped Bi 4 O 5 BrI (Ni/Bi 4 O 5 BrI-S), which demonstrates bulk-surface charge polarization and active site manipulation. Specifically, this bulk-surface charge polarization, resulting from a cascade of the bulk electric field (BEF) and local surface electric field (LSEF), induces efficient separation of bulk and surface charge carriers. Moreover, the atomically dispersed Ni sites substantially augment active sites for O 2 activation, further accelerating charge transfer and increasing the generation of photogenerated holes (h + ) and superoxide radical (•O 2 − ) active species for triggering efficient aerobic oxidation of sulfide. This study presents a collaborative strategy for manipulating charge behavior with potential applications in renewable energy and green chemistry.
研究领域:
材料科学
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有机合成
·
绿色化学
✓ 已验证
产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2020
·Vol. 11
·期 1
·297-311
·
IF 5.721
Xiaoqiang Zhang,Peifang Yan,Bin Zhao,Z. Conrad Zhang
The electronic and structural differences of anatase TiO2 (TiO2-A) and rutile TiO2 (TiO2-R) supported Ni catalysts are studied to understand the distinctively different catalytic pathways in guaiacol hydrodeoxygenation over Ni/TiO2-A and Ni/TiO2-R catalysts. Temperature programmed reduction profiles of NiO/TiO2-A and NiO/TiO2-R reveal two types of metal–support interactions. NiO on TiO2-R requires much higher temperature to reduce than NiO on TiO2-A by hydrogen reduction. Surface TiO2-A is partially reduced together with NiO at low temperature driven by strong interaction between reduced Ni and the reducible TiO2-A surface. In situ X-ray photoelectron spectroscopy (XPS), high resolution TEM (HRTEM), and diffuse reflectance infrared Fourier transform (DRIFT) spectroscopy of adsorbed CO reveal two types of reduced Ni species on Ni/TiO2-A: Ni0 particles and atomically dispersed electron-rich Niδ− atoms. While Ni0 particles are formed only at high Ni loadings, they are fully encapsulated by an overlayer of partially reduced TiOx, making the surface of Ni particles totally inaccessible to CO and to reactants. The electron-rich Niδ− atoms are favorably formed at all Ni loadings on the TiO2-A surface and show only linearly adsorbed CO in the DRIFT spectra. Electron transfer from Ti and O on the TiO2-A surface to atomically dispersed Ni is indicated by the observation of dominant electron-rich Niδ− species in conjunction with Ti(4+δ)+ and O(2−δ)− on Ni/TiO2-A following H2 reduction. In contrast, the chemical states of metallic Ni0 and Ti4+ remain unchanged on Ni/TiO2-R after H2 reduction. The atomically dispersed Niδ− species, formed only on the Ni/TiO2-A surface, is proposed as the active site responsible for the selective hydrodeoxygenation of guaiacol to phenolics. In contrast, the metallic Ni0 particles formed on the Ni/TiO2-R surface catalyze the typical catalytic hydrogenation, preferentially saturating the aromatic ring.
研究领域:
化学
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材料科学
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催化反应
✓ 已验证
DOI
高影响因子
Sustainable Energy & Fuels
·
2024
·Vol. 8
·期 13
·2860-2868
·
IF 5
Lan-Hui Feng,Zhi-Hui Lv,Yi-Jie Kong,Xin-Ming Hu
Excessive CO2 emission and plastic waste pollution constitute two pressing threats to our environment. Effective tactics are urgently demanded to address these issues. Herein, we report that the thermal treatment of plastic wastes in the presence of nickel chloride, melamine, and KCl/LiCl salt mixture produces atomic nickel and nitrogen-doped carbon materials (Ni–N–C), which are proven to be effective for electrocatalytic CO2 conversion. We disclose that the treating temperature and the activation of molten KCl/LiCl play critical roles in fabricating Ni–N–C with high porosity, abundant Ni sites, and good charge transfer ability. As a result, Ni–N–C-800 prepared from polyethylene terephthalate bottles exhibits good performance in electrochemical CO2-to-CO conversion. Importantly, a large current density of 400 mA cm−2 and a high faradaic efficiency of 90% for CO production can be achieved in the flow cell, which endows Ni–N–C-800 with great prospects for industrial applications. Furthermore, we show that the thermal treatment of other plastic wastes such as polyethylene, polypropylene, and polyvinyl chloride can also yield effective Ni–N–C catalysts, demonstrating good universality of upcycling plastic wastes to efficient catalysts. This study puts forward a sustainable solution for the simultaneous valorization of both CO2 and plastic wastes.
研究领域:
环境科学
·
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）