JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2020
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IF 7.489
Wei Wang,Yunlei Zhong,Xinyu Zhang,Sainan Zhu,Yourong Tao,Yanxin Zhang,Hongsen Zhu,Yifei Zhang,Xingcai Wu,Guo Hong
Surface self-reconstruction by the electrochemical activation is considered as an effective strategy to increase the oxygen evolution reaction (OER) performance of transition metal compounds. Herein, uniform Co 2 (OH) 3 Cl microspheres are developed and present an activation-enhanced OER performance caused by the etching of lattice Cl − after 500 cyclic voltammetry (CV) cycles. Furthermore, the OER activity of Co 2 (OH) 3 Cl can be further enhanced after small amounts of Fe modification (Fe 2+ as precursor). Fe doping into Co 2 (OH) 3 Cl lattices can make the etching of surface lattice Cl − easier and generate more surface vacancies to absorb oxygen species. Meanwhile, small amounts of Fe modification can result in a moderate surface oxygen adsorption affinity, facilitating the activation of intermediate oxygen species. Consequently, the 10% Fe-Co 2 (OH) 3 Cl exhibits a superior OER activity with a lower overpotential of 273 mV at 10 mA cm −2 (after 500 CV cycles) along with an excellent stability as compared with commercial RuO 2 .
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ACS Sustainable Chemistry & Engineering
·
2019
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IF 6.97
Wenrui Wan,Dazhen Xiong,Qian Zhang,Jianji Wang
It is very important to develop “smart” solvents that can integrate the advantages of homogeneous and heterogeneous reactions into one chemical process for enhanced reaction rate and minimal environmental impact. In designing these solvents, the applicability of the systems to real processes strongly depends on the phase behavior of the systems. In this work, a novel class of CO2-driven miscible–immiscible transition of deep eutectic solvents (DESs) has been explored. These DESs are composed of alkanolamine compounds as hydrogen-bond acceptors (HBAs) and phenolic compounds as hydrogen-bond donors (HBDs). They exhibit unique phase behavior with H2O: miscible with water in the absence of CO2 but immiscible with water in the presence of CO2 at room temperature and ambient pressure. Reversible liquid–liquid phase transition of such DES–H2O mixtures can be realized by alternative bubbling of CO2 and N2 under ambient conditions. Spectroscopic investigations show that the mechanism behind the miscible–immiscible transition of DESs involves breaking of the hydrogen bonds between HBDs and HBAs by H2CO3 generated by bubbling CO2 through an aqueous solution because the acidity of H2CO3 is stronger than that of HBAs. Further, the HBAs react with H2CO3 to form ammonium salts. The salting-out effect of ammonium salts leads to the formation of an ammonium salt-rich top phase and an HBD-rich bottom phase. When CO2 is removed by bubbling of N2, a reversible process is achieved.
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APPLIED SURFACE SCIENCE
·
2022
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IF 7.392
Gaosheng Ren,Zhihui Su,Yu Tang,Weichen Du,Nan Xu,Chengyi Dai,Xiaoxun Ma
It is very important to design model catalysts to control the site distribution and develop methods to improve their electronic environment and thus promote the catalyst’s performance in the electrochemical reduction of CO 2 (CO 2 RR). In this work, a strategy of in-situ synthesis and anchoring of nanoparticles (SSAN) was developed. Using this strategy, a “jujube-cake” type catalyst was designed, referred to as Ag@4-MBA. In this catalyst, Ag nanoparticles (NPs) act as “jujube”, which are embedded in 4-mercaptobenzoic acid (4-MBA) acting as “cake”. A Pointer-shaped Ag@4-MBA material was prepared that achieved high loading of Ag species (∼24.0 wt%), high dispersion (5–10 nm), high CO mass activity (93.7 A g Ag −1 ), high CO faradaic efficiency (94.0%) and high CO production (2.0 mol g Ag −1 h −1 ), showing a superior performance to that of the recently reported Ag-based catalysts. Density functional theory (DFT) calculations and X-ray photoelectron spectroscopy (XPS) characterization showed that a high degree of electron delocalization of the Ag–S–aromatic ring and reconstructing the electronic environment of the metal sites were achievied, it is beneficial to stabilize the reaction intermediate COOH*. This work provides a new approach for the design of metal nanoparticle model catalysts with more sustainable CO 2 RR.
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ELECTROCHIMICA ACTA
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2022
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IF 7.336
Shuyan Shao,Tao Wen,Ziqun Wang,Xiaoshuang Yin,Ying Liu,Wenzhong Yang,Yun Chen
Electrocatalytic reduction of CO 2 to formate is an extremely attractive route. Here, we developed a SnSe 2 -graphene composite catalyst, and SnSe 2 nanosheets were linked to graphene by Sn-O-C bonds to form complicated hierarchical nanosheet structure. Due to the intrinsic activity of SnSe 2 and the modification of graphene, the catalyst performed excellent electrocatalytic efficacy for the reduction of CO 2 to formate, with a maximum Faraday efficiency up to 95.1% at -0.9 V (vs. RHE) and a current density of 11.8 mA cm −2 under the optimal conditions. Kinetic experiments indicated that the SnSe 2 -graphene composite achieved efficient formate selectivity for CO 2 reduction by increasing the initial transfer rate of electrons to the CO 2 molecule.
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DALTON TRANSACTIONS
·
2022
·Vol. 51
·期 44
·17081-17088
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IF 4.569
Wenyuan Wang,Kai Zhang,Tao Xu,Yagang Yao
Nowadays, the goal of carbon peaking and carbon neutrality has become a global consensus, and electrochemical CO2 reduction to provide high-value power fuel is one of the major technical approaches attracting significant research interests and application prospects. However, the inevitable hydrogen evolution reaction in water-based electrolyte systems crowds out the reactive sites of active metals, causing a low CO2 conversion efficiency. In this work, Zn nanosheets were prepared via electrodeposition on the surface of carbon paper and then modified with polytetrafluoroethylene (PTFE) to tune the wetting angle of the electrolyte. A CO faradaic efficiency of 90.2% was achieved for Zn NS-8% PTFE (contact angle: 136.8°) at the electrolytic voltage of −1.0 V vs. RHE along with an overall current density of −7.9 mA cm−2. Experimental results and molecular dynamics simulation revealed that PTFE weakened the aggregation of H2O molecules and was more beneficial for capturing and adsorbing CO2 molecules near the electrode surface. The active sites of hydrogen production were transformed into the reaction center for electrocatalytic CO2 reduction due to the hydrophobicity of the electrode, and the accumulation of the local CO2 concentration accelerated the kinetic activity for electrochemical conversion (CO2 to CO). This strategy of tuning the local environment offers an alternative approach for effective electrode manufacturing in liquid electrolytes.
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ACS Catalysis
·
2026
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IF 13.6
Liu Meng-Nan,He Zhen-Hong,Chen Zhuo,Wang Sen-Wang,Ruan Miao,Luo Yanping,Wang Kuan,Wang Weitao,Wang Huan,Liu Zhao-Tie
Direct hydrogenation of CO 2 to liquid hydrocarbons (C 5+ ) at low temperature is a highly desirable but challenging transformation, as conventional catalysts typically operate at high temperatures via indirect pathways by producing and using a CO intermediate. In this work, we report an inverse ZrO 2 /Co catalyst that enables direct CO 2 hydrogenation to C 5+ hydrocarbons at a low temperature of 200 ° C. Under optimal conditions, the catalyst achieves a high CO 2 hydrogenation activity of 26.0 mmol CO2 ·g Co –1 ·h –1 with 58.9 C-mol % selectivity toward C 5+ liquid hydrocarbons and negligible CO formation. The inverse architecture of ZrO 2 /Co, wherein ZrO 2 nanoislands are dispersed over metallic Co 0 particles, concurrently not only enhances CO 2 adsorption and suppresses H 2 adsorption but also delivers a surface C/H ratio approximately 31 times higher than that of pristine Co 0 , thereby promoting chain growth. In situ DRIFTS reveals that the inverse catalyst generates abundant oxygen-containing intermediates (HCOO–, HCO 3 –, CH 3 O–, and CH 3 COO–), which are subsequently hydrogenated to CH x for chain growth over Co 0 sites. This work not only provides a low-temperature catalyst for direct CO 2 -to-C 5+ conversion but also establishes inverse oxide/metal interfaces as a general platform for tuning C–C bond coupling in CO 2 hydrogenation.
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JOURNAL OF CATALYSIS
·
2023
·
IF 7.3
Zemin An,Nan Ma,Yuanjie Xu,Hua Yang,Huibo Zhao,Lizhi Wu,Li Tan,Chao Zou,Fanchun Meng,Bin Zhang,Xiuyun Wang,Yu Tang
Harnessing the selectivity in catalytic hydrogenation of CO 2 is important for producing valuable chemicals. Herein, the shape dependency of the CO 2 hydrogenation on singly dispersed Ru/CeO 2 catalysts is investigated. CeO 2 of three shapes, including nanocube, nanooctahedron and nanorod, are prepared as the catalyst supports and assigned to the surface of (100), (111) and (110) crystal plane, respectively. The Ru/CeO 2 (nanorod) exhibits the highest selectivity to CO (97.6 %) at 350 °C, while the Ru/CeO 2 (nanocube) exhibits a mediocre selectivity to CO (41.4 %) but the highest CO 2 conversion. The shape of the CeO 2 support determines the electronic state of supported Ru atoms through the electronic metal-support interaction. The low CO affinity on cationic Ru β sites leads to the higher selectivity to CO on the Ru/CeO 2 (nanorod) and Ru/CeO 2 (nanooctahedron) catalysts, while the strong dissociation ability of H 2 on low valence Ru α sites results in the high activity on the Ru/CeO 2 (nanocube) catalyst.
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CHEMICAL ENGINEERING SCIENCE
·
2023
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IF 4.7
Tiantian Chen,Min Zhou,Zhiquan Zhang,Kai Yang,Xiaohong Fu,Huaming Li,Weidong Shi,Zhifeng Jiang
CO 2 Photoreduction through C–O bond cleavage and C–H bond formation has aroused as an alternative to fabricate high-value chemical fuels that are independent of fossil reserves. However, sluggish charge transfer and neglected light-induced heat utilization are thermodynamically and kinetically challenging. Herein, we subtly design a three-dimensional ultrathin composite consisting of flower-like ZnIn 2 S 4 (ZIS) and low-cost biochar (BC). The as-prepared ZIS/BC photocatalyst displays an optimized performance and stability toward CO 2 conversion, with a high CO yield of 20.7 μmol g −1 h −1 and a small yield of CH 4 , C 2 H 4 , and C 2 H 6 in comparison with ZIS and BC counterparts. This exciting activity originates from high electron conduction efficiency, light-harvesting ability, and the photothermal effect, which is produced from the intense interfacial contact of BC and ZIS. This work suggests that traditional photocatalysts can be elevated by inhibiting photocorrosion by introducing highly economical and electron conductivity biomass carbon in solar-induced green-chemical feedstock production.
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Molecular Catalysis
·
2023
·
IF 4.6
Zhishuai Wang,Fengyun Su,Hailong Cao,Mengzhen Tian,Xiang Li,Haiquan Xie,Xiaoli Jin,Zhengdao Li,Xin Ying Kong
Amidst the impending energy crisis and escalating concerns about global warming, photocatalytic reduction of carbon dioxide (CO 2 ) emerges as a promising solution. However, the practical application of this technology has been hindered by challenges such as the poor photoresponse of existing photocatalysts toward visible light, inefficient separation efficiency of photoinduced electron-hole pairs, and subpar product selectivity. This work simultaneously addresses these limitations by enhancing the activity of photocatalytic CO 2 reduction through the strategic incorporation of nickel oxide (NiO) onto niobium pentoxide (Nb 2 O 5 ). In this study, Nb 2 O 5 was prepared using the hydrothermal and calcination methods, culminating in the synthesis of NiO-supported Nb 2 O 5 achieved through the photodeposition method. The resulting 2 %-NIONBO photocatalyst with the optimal loading of NiO exhibited a remarkable methane (CH 4 ) production yield of 29.65 μmol/g/h, a striking 6.2-fold improvement over solitary NBO. In addition, the useful carbon monoxide (CO) fuel was also detected from the photoreduction of CO 2 , where 2 %-NIONBO exhibited a CO yield of 7.22 μmol/g/h, demonstrating a 3.4-fold enhancement over NBO, along with an outstanding CH 4 selectivity of 80.42 %. This study provides insights into the design and development of Nb-based photocatalysts for significantly enhanced efficiency in photocatalytic CO 2 reduction, paving the way for advancements in sustainable energy solutions and addressing environmental issues.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-12
·
IF 16.6
Jiao Jiqing,Yuan Qing,Tan Meijie,Han Xiaoqian,Gao Mingbin,Zhang Chao,Yang Xuan,Shi Zhaolin,Ma Yanbin,Xiao Hai,Zhang Jiangwei,Lu Tongbu
Elucidating the synergistic catalytic mechanism between multiple active centers is of great significance for heterogeneous catalysis; however, finding the corresponding experimental evidence remains challenging owing to the complexity of catalyst structures and interface environment. Here we construct an asymmetric TeN 2 –CuN 3 double-atomic site catalyst, which is analyzed via full-range synchrotron pair distribution function. In electrochemical CO 2 reduction, the catalyst features a synergistic mechanism with the double-atomic site activating two key molecules: operando spectroscopy confirms that the Te center activates CO 2 , and the Cu center helps to dissociate H 2 O. The experimental and theoretical results reveal that the TeN 2 –CuN 3 could cooperatively lower the energy barriers for the rate-determining step, promoting proton transfer kinetics. Therefore, the TeN 2 –CuN 3 displays a broad potential range with high CO selectivity, improved kinetics and good stability. This work presents synthesis and characterization strategies for double-atomic site catalysts, and experimentally unveils the underpinning mechanism of synergistic catalysis.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
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IF 4.2
Lei Yuan,Leihao Zhang,Guilin Li,Shaojuan Zeng,Qizhou Xue,Chongyang Jiang,Xiangping Zhang
Electric-driven reduction of CO2 to high value-added chemicals is considered to be one of the most promising methods for CO2 utilization. In this work, a novel aprotic electrolyte consisting of phenoxy-nitrile bifunctional ionic liquid ([TBP][p-CN-PhO]) and acetonitrile was designed for CO2 electroreduction to oxalate, which shows the maximum Faradaic efficiency (FE) of 84.9% at −2.6 V. Importantly, a high oxalate formation rate of 233.7 μmol·cm–2·h–1 and oxalate FE of 73.9% were simultaneously achieved to break the trade-off effect at −2.8 V in the bifunctional ionic liquid electrolyte, which is also one of the state-of-the-art performances for CO2 electroreduction to oxalate. The significant performance of CO2 electroreduction was attributed to the strong interaction energies of phenoxy and nitrile groups with CO2 molecules in the bifunctional ionic liquid, which greatly facilitates CO2 activation to form CO2– radicals by a new bulk-phase pathway and then dimerizes into C2O42– at a lower energy barrier.
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ACS Applied Nano Materials
·
2023
·
IF 5.9
Xiaoqian Peng,Jing Zhang,Jinqiang Sun,Xiaochan Liu,Xinfu Zhao,Shimo Yu,Zhipeng Yuan,Sijia Liu,Xibin Yi
One of the most promising methods for capturing carbon dioxide (CO2) is solid physical adsorption, which is an efficient and simple technique. The key to effective CO2 capture is the development of high-performance solid adsorbents with excellent CO2 adsorption capacity, CO2/N2 selectivity, and rapid adsorption/desorption kinetics. In this paper, a Mg-MOF-74/sodium alginate composite aerogel was prepared by loading Mg-MOF-74 on sodium alginate sheets followed by directional freeze-drying. The composite aerogel exhibited a hierarchical porous structure, in which sodium alginate provided an open mesoporous/macroporous structure that promoted diffusion and contact with the active center of CO2. The Mg-MOF-74 micropores/mesopores promoted the strong interaction between CO2 and the adsorbent in the micropore and rapid mass transfer of CO2 to the adsorbent through the mesopores. The experimental data showed that MSA-6 achieved CO2 adsorption of 2.461 mmol·g–1 at 298 K. Furthermore, the CO2/N2 adsorption selectivity of MSA-6 reached 35.108, indicating its strong CO2 selective adsorption potential.
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