iScience
·
2023
·
IF 5.8
Qing Zhang,Chen Fang,Yanlan Wang,Xiang Liu
Summary In the winter months, the temperature in most of the Earth stays below 0°C; the average temperature in winter at the South Pole is about −60°C. Therefore, it is urgent to develop efficient catalytic systems for selective and efficient H 2 evolution upon NH 3 BH 3 hydrolysis at subzero temperatures. For solving the freezing issue of water at below 0°C, herein, we have employed a facile and surfactant-free approach to synthesize M-Pt/C nanocomposites (M = Pd, Rh, Ru, Ni, Cu, or Fe), by the alloying of commercial Pt/C with Pd, Rh, Ru, Cu, Ni, or Fe for selective and efficient H 2 evolution upon NH 3 BH 3 hydrolysis in saline solution at below 0°C, even at −15°C. In addition, NH 3 BH 3 hydrolysis over Pd-Pt/C in the saturated NaCl solution is utilized not only for safe hydrogen production but also for its in situ hydrogenation reduction in organic chemistry, which could avoid using dangerous hydrogen cylinders.
研究领域:
化学
·
材料科学
·
能源研究
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Wenjie Xue,Binbin Zhao,Hongxia Liu,Xinqing Chen,Lei Liu
The facile catalytic reversible (de)hydrogenation of liquid organic hydrogen carriers (LOHC) using a single catalyst holds great value for onboard hydrogen storage. Herein, we develop a bimetallic catalyst Pd 1 Ni based on nonnoble metal Ni with ultralow Pd of 0.05 wt%, which enables reversible (de)hydrogenation of NPC and supports multiple cycles of reversible hydrogen uptake and release. Notably, the bimetallic catalyst Pd 1 Ni exhibits more excellent catalytic performance on the dehydrogenation reaction of dodecahydro-N-propylcarbazole (12H-NPC) than the 1%Pd catalyst and similar catalytic performance on the hydrogenation reaction of NPC compared to the 1%Ru catalyst. The astonishing catalytic efficiency of Pd 1 Ni catalysts is due to the ideal electronic structure between ultralow Pd and Ni NPs allowing rapid interfacial electron transfer to intermediates, as revealed by structural analyses and density functional theory (DFT) computations.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2024
·
IF 6.5
Jianguo Wu,Haoxiang Xu,Dong Cao,Daojian Cheng
Supported PdAu bimetallic nanoparticles have been developed for the direct synthesis of H 2 O 2 (DSHP). However, to date, the dilute H 2 streams necessary to avoid potential risks of explosion limits the attainable product concentrations of H 2 O 2 . Here, a series of silicon-modified Al 2 O 3 (Si x Al) were synthesized for loading PdAu bimetallic nanoparticles . The H 2 consumption turnover frequency (TOF) and H 2 O 2 formation TOF show a volcano trend with the silica content, where PdAu/Si 5.6 Al exhibits the best H 2 consumption TOF and H 2 O 2 formation TOF (11259.3 and 1995.2 h −1 ). Silica on the surface of Al 2 O 3 is identified as Brønsted (B) acid site. The increase of B acid sites density accelerates the H 2 conversion into H atoms, thereby boosting H 2 O 2 formation process. The adsorption and dissociation of H 2 into atomic H at B acid sites would spill across the support to PdAu nanoparticles reversely. The reversed hydrogen spillover effect induced by B acid site accounts for enhanced H 2 conversion and H 2 O 2 productivity for PdAu/Si x Al.
研究领域:
催化
·
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Xia Bai,Jingmin Ge,Huanhuan Yang,Huiwen Tian,Xueqi Liu,Shiying Li,Zhikun Peng,Yaxi Li,Jiahao Wang,Hongpo Liu,Qun Xu
Building of grain boundary (GB) in Cu-based catalysts has been demonstrated to be an efficient strategy to control the product selectivity of electrochemical CO 2 reduction reaction (eCO 2 RR). However, the fabrication and modulation of GBs in Cu are still challenging. In this study, a series of bare Cu catalysts with controllable density of Cu(111) GBs were investigated systematically for eCO 2 RR. These catalysts exhibit superior eCO 2 RR performance for syngas production with a high FE of ∼80 % and tunable H 2 /CO ratio of 0.46–2.78. Three-dimensional wormlike Cu with abundant (111) GBs displays a stable H 2 /CO ratio of ∼0.5 over a wide potential range from −0.9 to −1.2 V ( vs. RHE). In situ Raman and ATR-SEIRAS spectroscopy combined with DFT calculations reveal that Cu(111) GBs enhance the adsorption of CO 2 , lower the energy barriers of CO 2 to *COOH and *CO, further highlighting the potential to control syngas production with desirable proportion over Cu-based catalysts.
研究领域:
材料科学
·
电化学
·
催化
·
能源转化
✓ 已验证
DOI
高影响因子
Reaction Chemistry & Engineering
·
2022
·Vol. 8
·期 1
·64-76
·
IF 5.2
Haosheng Xin,Haiyong Wang,Xiaohong Hu,Xiuzheng Zhuang,Long Yan,Chenguang Wang,Longlong Ma,Qiying Liu
Cellulose hydrolysis and further conversion to diketones and alcohols was performed with graphene layer encapsulated cobalt catalysts (Co@C) in phosphoric acid aqueous solution. A total of 60.5% yield of the products mainly including ethanol, 2,5-hexanedione (2,5-HD) and diols could be achieved in 0.06 M H3PO4 solution. A series of characterization methods such as XRD, XPS, TEM, TG-MS, BET, ICP, H2-TPD, NH3-TPD, and Raman were carried out to explore the catalyst formation mechanism and reaction activity. The results of the analysis indicated that the calcination temperature had a deep influence on the structure formation of the Co@C catalysts, thus leading to differences in the reaction activity. While the calcination temperature was determined at 700 °C, the Co@C catalyst meets with the requirements of optimal reaction activity, appropriate particle size, suitable surface area, and pore size. Besides, it was found that H3PO4 is not only favorable in cellulose hydrolysis but also cooperates with the Co@C catalyst in the hydrogenolysis of C–O bond and C–C bonds for the formation of products. This work provides a possible way for renewable cellulose conversion to diketone and alcohols over encapsulated non-noble metal catalyst combined with phosphoric acid aqueous solution.
研究领域:
化学工程
·
催化
·
可再生能源
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2021
·Vol. 11
·期 20
·12022-12029
·
IF 3.361
Zhuo Jia,Rong Dai,Ziliang Zheng,Yufei Qin,Ailin Duan,Xiaoyang Peng,Xianmei Xie,Ruiping Zhang
Compared with the near-infrared-I spectral window (NIR-I, 650–950 nm), a newly developed imaging and treatment window with a 1000–1700 nm range (defined as the NIR-II bio-window) has attracted much attention owing to its higher spatiotemporal resolution, increased tissue penetration depth and therapeutic efficacy. Herein, we designed a nanotheranostic platform (HC-AB NPs) via loading ammonia borane (AB) into hollow carbon nanoparticles (HCs) for NIR-II photoacoustic (PA) imaging-guided NIR-II hydrogenothermal therapy. Importantly, by exploiting the characteristics of beta zeolite as a hard template and a template-carbonization-corrosion process, the prepared HCs have excellent NIR-II absorption performance and AB loading capacity. With the high biocompatibility of HC-AB NPs, an efficient synergistic anti-tumor strategy has been achieved via high intratumoural accumulation and acid-stimulated H2 release as well as PA-guided precise NIR-II photothermal therapy. The HC-AB NPs as a promising nanotheranostic platform opens a new avenue for high-efficacy NIR-II hydrogenothermal therapy.
研究领域:
生物医学工程
·
纳米技术
·
癌症治疗
·
成像技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
FUEL PROCESSING TECHNOLOGY
·
2023
·
IF 7.5
Yuanling Li,Han Yu,Jing Dai,Zhenzong Zhang,Zhichao Zhang,Hongbing Yu,Lina Liu
Non-thermal plasma (NTP) combined with catalysts supplies a potential alternative to enable the CH 4 and CO 2 conversion to work at low temperatures. In this study, different Ni/BN catalysts were synthesized using modified wetness impregnation for CH 4 and CO 2 conversion in dielectric barrier discharge (DBD) plasma. Among, BN_IPA_Ni exhibited the highest catalytic performance with a CH 4 conversion of 40.5%, a CO 2 conversion of 26.6%, a H 2 yield of 9.3% and a CO yield of 10.5%. The development of B O defects, which played a significant role in the size control of Ni particles to facilitate the dissociation of CH 4 to form H*, is the key for the high catalysis activity and selectivity in this reaction. In addition, the B O defects of BN_IPA_Ni provide an efficient route to eliminate excess CH x species, which further inhibit the nucleation growth of carbon species to inert carbon.
研究领域:
化学工程
·
催化
·
等离子体化学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
2025
·
IF 13.1
Yingqiao Zhou,Bowen Yang,Richard L Smith Jr.,Yaqiong Su,Xinhua Qi
The development of recyclable heterogeneous bifunctional catalysts for the efficient conversion of cellulose into high-value platform chemicals is still a significant challenge. Herein, the preparation of carbon-nanosheet-encapsulated nickel phosphide catalysts was performed via solvent evaporation self-assembly and alkali activation, and the as-synthesized catalyst efficiently (3 h) hydrolyzes and hydrogenates microcrystalline cellulose to sorbitol with a sorbitol yield exceeding 90%. As a bifunctional catalyst, nickel phosphide (Niδ+–Pδ–) facilitates the heterolytic cleavage of H2, simultaneously generating in situ acidic Hδ+ species for hydrolysis and hydridic Hδ– species for the hydrogenation of C═O bonds. Unlike conventional catalysts with spatially separated functionalities, this concurrent process avoids intermediate accumulation and side reactions during cellulose conversion. Furthermore, encapsulation by carbon nanosheets suppresses phosphorus leaching under hydrothermal conditions, endowing the catalyst with balanced durability and activity. This work provides fundamental insights into hydrogen activation by transition metal phosphides and advances the design of bifunctional catalysts integrating both acidic and hydrogenation functionalities.
研究领域:
催化
·
可再生能源
·
生物质转化
·
材料科学
·
多相催化
✓ 已验证
产品关联
DOI
高影响因子
INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Jing Xu,Xueqi Zhang,Wei Yan,Tengfeng Xie,Yuanping Chen,Yingcong Wei
It is highly desirable but challenging to optimize the electronic structure of an active site to realize moderate active site-Hads bond energies for boosting photocatalytic H2 evolution. Herein, an interfacial engineering strategy is developed to simultaneously concentrate hydrogen species and accelerate the combination of an Hads intermediate to generate free H2 by constructing W–WC–W2C (WCC) cocatalysts. Systematic investigations reveal that hybridizing with W2C creates electron-rich W active sites and effectively induces the downshift of the d-band center of W in WC. Consequently, the strong W–Hads bonds on the surface of WC are weakened, thus promoting the desorption of Hads to rapidly produce free H2. The optimized 40-WCC/CdS photocatalyst exhibits a high hydrogen evolution rate of 63.6 mmol g–1 h–1 under visible light (≥420 nm) with an apparent quantum efficiency of 39.5% at 425 nm monochromatic light, which is about 40-fold of the pristine CdS. This work offers insights into the design of cocatalyst for high-efficiency photocatalytic H2 production.
研究领域:
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
FUEL
·
2024
·
IF 6.7
Mengjie Cao,Shuangde Li,Shikun Wang,Weichen Xu,Xin Zhou,Guangxin Ma,Xiaoze Wang,Linfeng Nie,Yunfa Chen
Designing nickel-based methane cracking catalysts with excellent catalytic activity and surveying their transition during the catalytic process with varied reaction condition have been challenge. In this paper, NiAl catalysts were prepared by reduced hydrotalcite precursor for efficient catalytic methane cracking to produce hydrogen. The catalysts were characterized by XRD, N 2 physisorption, XPS, SEM, TEM, Raman and TGA. The effects of preparation method, Ni/Al ratio and reaction temperature on methane cracking performance were revealed and the transformation for the Ni particles during the reaction process was analyzed. The results indicated that the catalyst performance of hydrotalcite-derived NiAl catalysts is superior to Ni/Al 2 O 3 catalysts prepared by the conventional impregnation method, which maybe due to the better Ni dispersion and uniform average particle size distribution with around 12.7 nm compared with the agglomeration of the Ni/Al 2 O 3 particles for up to 53.2 nm. The catalyst with a Ni/Al molar ratio of 3 exhibited the optimal catalytic activity with a stability for 75 min at nearly 90 % hydrogen yield at 700 °C. The reaction temperature also suggested a positive correlation between the hydrogen yield and the reaction temperature from 600 °C to 800 °C. Moreover, based on the investigation of the catalysts during the reaction transition state, Ni particles sintered rapidly from 10.2 nm to 31.2 nm at the beginning reaction time with the high hydrogen yield and then tended to be stable, which may be correlated well with the degree of graphitization of the deposited carbon. This paper provides a valuable design for efficient methane cracking catalysts.
研究领域:
催化
·
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Research
·
2021
·
IF 0
Yao Chen,Dong Yang,Yuchen Gao,Runlai Li,Ke An,Wenjing Wang,Zhanfeng Zhao,Xin Xin,Hanjie Ren,Zhongyi Jiang
The rational design of an outer shell is of great significance to promote the photocatalytic efficiency of core-shell structured photocatalysts. Herein, a covalent organic framework (COF) nanoshell was designed and deposited on the cadmium sulfide (CdS) core surface. A typical COF material, TPPA, featuring exceptional stability, was synthesized through interfacial polymerization using 1, 3, 5-triformylphloroglucinol (TP) and p-phenylenediamine (PA) as monomers. The nanoshell endows the CdS@TPPA nanosphere with ordered channels for unimpeded light-harvesting and fast diffusion of reactants/products and well-defined modular building blocks for spatially charge separation. Moreover, the heterojunction formed between CdS and TPPA can further facilitate the effective charge separation at the interface via lower exciton binding energy compared with that of pristine TPPA. By modulating the thickness of TPPA nanoshell, the CdS@TPPA nanosphere photocatalyst with the nanoshell thickness of about 8±1 nm exhibits the highest photocatalytic H2 evolution of 194.1 μmol h-1 (24.3 mmol g-1 h-1, 8 mg), which is superior to most of the reported COF-based photocatalysts. The framework nanoshell in this work may stimulate the thinking about how to design advanced shell architecture in the core-shell structured photocatalysts to achieve coordinated charge and molecule transport.
研究领域:
材料科学
·
能源化学
·
光催化技术
✓ 已验证
DOI
ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Zichao Lian,Ying Tao,Yunni Liu,Yang Zhang,Qiong Zhu,Guisheng Li,Hexing Li
The photoelectrocatalytic (PEC) technique has attracted much attention to getting clear energy and environmental purification. Simultaneous reactions of solar energy generation could be used to apply for practical applications to maximize the functionality of reactor systems. Herein, we crafted a self-driving photoelectrocatalytic reactor system, comprising platinum (Pt) modified p-Si nanowires (Pt/Si-NWs) as a photocathode and TiO2 nanotube arrays (TiO2–NTAs) as a photoanode for synergistic H2 evolution and water purification, respectively. Hydrogen evolution in the cathode chamber and environmental remediation in the anode chamber were achieved with the aid of appropriate bandgap illumination and self-built bias voltage. The mismatch of Fermi levels between TiO2–NTAs and Si-NWs reduced the recombination rates of photoinduced electrons and holes through the formation of Z scheme and inner electric filed. The synergistic PEC reactions exhibited much higher activities than those achieved using other systems so far. This basic principal could be applied for fabricating other PEC reactors in photoelectro conversion devices and be established as design guidelines for reactors to maximize the PEC performance.
研究领域:
环境科学
·
材料科学
·
能源科学
✓ 已验证
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）