INTERNATIONAL JOURNAL OF ENERGY RESEARCH
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2022
·Vol. 46
·期 12
·17015-17028
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IF 4.672
Xueliang Sun,Qilong Wang,Yuyu Liu,Jin Yi,Jiujun Zhang
Summary CO 2 reduction to produce value-added chemicals/fuels is generally considered as an effective way to solve the energy crisis and global warming. However, the greatest challenge to the technology is the lack of high-performance catalysts as this process is quite sluggish under mild conditions. Herein, we have carefully prepared a series of bimetallic Pb x Cd y nanoparticles (NPs) as well as their monometallic counterparts via a facile chemical reduction. Electrocatalytic performances of obtained catalysts were evaluated with respect to chemical composition, electrolytic potential, and so on. All of them exhibit high performance and achieve high faradaic efficiency for HCOOH production (FE HCOOH ) over a voltage window of −1.16 to −1.26 V vs the reversible hydrogen electrode (V RHE ). Among them, Pb 3 Cd 1 achieved a maximum FE HCOOH of 96% at −1.16 V RHE and a desirable stability over 12 hours of continuous electrolysis. The excellent performance of Pb 3 Cd 1 can be attributed to the huge specific area of NPs and the synergistic effect of the components. This study shows that efficient bimetallic Pb x Cd y electrocatalysts have a large application potential for highly selective HCOOH production from CO 2 . Highlights Bimetallic PbCd nanoparticles were synthesized by facile chemical reduction for electrocatalytic CO 2 reduction. PbCd nanocatalysts performed well in highly active, selective, and stable HCOOH electrosynthesis from aqueous CO 2 . Pb 3 Cd 1 achieved maximum HCOOH faradaic efficiency of 96% at −1.16 V RHE , a record as far as we know. A stable current density (>7 mA cm −2 ) can be kept after a 12-hours continuous electrolysis.
研究领域:
材料科学
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环境科学
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化学工程
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
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IF 9.4
Yan Zheng,Pengting Sun,Shuxia Liu,Wenzheng Nie,Huihui Bao,Linglan Men,Qing Li,Zhongti Su,Yangyang Wan,Changlei Xia,Huan Xie
Electrochemical CO 2 reduction (ECO 2 R) to value-added chemicals offers a promising approach to both mitigate CO 2 emission and facilitate renewable energy conversion. We demonstrate a solar energy powered ECO 2 R system operating at a relatively large current density (57 mA cm −2 ) using In 2 O 3 nanosheets (NSs) as the cathode and a commercial perovskite solar cell as the electricity generator, which achieves the high solar to formate energy conversion efficiency of 6.6 %. The significantly enhanced operative current density with a fair solar energy conversion efficiency on In 2 O 3 NSs can be ascribed to their high activity and selectivity for formate production, as well as the fast kinetics for ECO 2 R. The Faradic efficiencies (FEs) of formate In 2 O 3 NSs are all above 93 %, with the partial current density of formate ranging from 2.3 to 342 mA cm −2 in a gas diffusion flow cell, which is among the widest for formate production on In-based catalysts. In-situ Raman spectroscopy and density functional theory simulations reveal that the exceptional performances of formate production on In 2 O 3 NSs originates from the presence of abundant low coordinated edge sites, which effectively promote the selective adsorption of *OCHO while inhibiting *H adsorption.
研究领域:
能源化学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Hao Jiang,Lizhang Wang,Bai Gao,Yiran Li,Yadan Guo,Mengning Zhuo,Kaixuan Sun,Binyu Lu,Meiyu Jia,Xiaoxia Yu,Huidong Wang,Yongge Li
In order to achieve high energy-conversion efficiency during CO 2 electro-conversion, OH − oxidation was employed as a counter reaction vs . CO 2 electroreduction for formate production on a Tin cathode. The formate faradic efficiency (FE) and production rate were 80.54% and 0.1549 mmol h −1 cm −2 using KOH anolyte at −1.80 V vs . SCE in 8 h operation, which were about 13.71% and 53.03% higher than that for KHSO 4 anolyte, respectively. This is mainly due to alkaline anolyte is beneficial to stabilize the catholyte pH, thus avoiding the competitive hydrogen evolution reaction, while maintaining fast electron transfer rate for the formation of CO 2* − . Moreover, KOH anolyte achieved the lowest power consumption (4.81 kWh kg −1 formate) compared with KHCO 3 and KHSO 4 . Polarization and electrochemical impedance spectroscopy measurements indicated that such energy-saving performance enhancement originated from low equilibrium potential and fast oxidation kinetics associated with the conversion of OH − to H 2 O, which reduced the anode potential and cell voltage. This study puts forward another insight for cost-effective CO 2 reduction, which is of great value to improve the balance of energy input and output during CO 2 conversion, thus having implication in enriching strategy in the field of electroreduction.
研究领域:
化学工程
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环境科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Hao Chen,Jia Song,Xin Long,Huanhua You,Yanhong Weng,Danni Liu,Yuanfeng Liao,Jiujun Zhang,Jing-Li Luo,Xian-Zhu Fu
It remains challenges to efficiently convert carbon-based fuels such as methanol from CO 2 into electrical energy while without CO 2 greenhouse gas emission. Herein, a CO 2 -emission free direct methanol fuel cell (DMFC) has been realized through using unique Pt-CoOOH/nickel foam anode with high electro-catalytical selectivity, activity and stability. The DMFCs demonstrate simultaneous production of 18 mol of formate for every 1 kWh of electricity output with peak power density of 49.3 mW cm −2 and high selectivity of formate value-added chemicals up to 96 %. Moreover, this simple procedure does not consume energy while output electricity compared to the traditional formate production. It either does not use the toxic feedstock of CO and the reaction conditions are very mild. The in-situ Raman test indicates that CoOOH acts as an auxiliary active site to promote the conversion of *HCO to *HCOOH and improve the selectivity of formate. In-situ IR tests and density functional theory (DFT) calculations confirm that methanol tends to be oxidized selectively into formate rather than complete-oxidizing into CO 2 . This study achieves clean and efficient utilization of carbon-based fuels to co-generate electrical energy and value-added chemicals while no CO 2 greenhouse emission, even realize the “negative carbon” cycle.
研究领域:
能源科学
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环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL TECHNOLOGY
·
2023
·
IF 2.8
Yuwei Zhang,Hengxi Zhu,Junjiang Guo,Weizhen Liu,Jiang Qi,Guan Qingqing,Bin Li,Ping Ning
In response to the social goal of ‘carbon peak and carbon neutral’ in the 14th Five-Year Plan of China, this article used Enrofloxacin (ENR), a common antibiotic, as a model compound to study the method of efficiently degrading pharmaceutical sludge and simultaneously producing Formic Acid (FA), hydrogen storage energy, in a sub-supercritical system. The Ni/SnO2 bimetallic catalyst, which was prepared by the equal volume impregnation method, was used for the liquid phase catalysis. As shown by the results, when the reaction temperature was 330°C, and the addition amount of H2O2 was 0.38 mL, the degradation rate of antibiotics could reach 99% after the reaction proceeded for 6 h. In terms of the resource utilization, the yield of FA could reach up to 32.44%. The resource utilization efficiency with Ni/SnO2 catalyst in sub-/supercritical reaction was about 2.5 times higher than that without catalyst. The kinetic reaction model was established to explore the reaction rate of the antibiotic degradation process. In addition, the Ea and the frequency factor of the reaction were 6455 J/mol and 5.78, respectively. As shown by characterization, the prepared Ni/SnO2 bimetallic catalyst had good activity and has already passed repeated stability experiments. In short, this method has broad application prospects in antibiotic catalysis and resource degradation.
研究领域:
环境科学
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催化化学
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能源化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
FUEL
·
2025
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IF 7.5
Honglin Li,Xin Zhang,Yuanyuan Wen,Jingyuan Li,Yu Liu,Hongjun Mao,Hongman Sun,Jingbin Zeng,Zifeng Yan
Sulfur-doped copper (S-doped Cu) was regarded as an efficient catalyst for formate in CO 2 electrochemical reduction reaction (CO 2 RR), but the selectivity and current density are still unsatisfied due to the hydrogen evolution reaction (HER) and CO generation pathway. Herein, S-doped Cu nanoparticles were synthesized by in-situ reduction of the constructed Cu-thioamide coordination polymers, exhibiting impressive performance for formate production in the CO 2 RR process. Particularly, the CuBr-thiobenzamide (TBA) coordination polymers derived S-doped Cu nanoparticles (CuBr-TBA-R) achieve a formate Faradaic efficiency of 84.4 % with current density of formate to 6.7 mA cm −2 . The characterization results indicate these generated S-doped Cu nanoparticles are uniform with the particle size of 20–30 nm exposed a large amount of Cu (100) facets due to the coordination of thioamide molecules and presence of Br - and I - in electrolyte. The morphological characteristics and strong affinity for oxygen is the reason of higher formate selectivity and current density. This finding reveals the characterizations of efficient S-doped Cu catalysts for formate and provide a controllable approach to prepare these catalysts.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
Frontiers of Chemical Science and Engineering
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2024
·Vol. 18
·期 11
·1-11
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IF 4.3
Gao Huimin,Zhang Jinpeng,Zhang Fangyuan,Jing Jieying,Li Wen-Ying
The photocatalytic reduction of CO 2 into formic acid is a feasible approach to alleviate the effects of global climate change and achieve chemical energy storage. It is important to design highly active photocatalysts to improve the selectivity and yield of formic acid. In this study, TiO 2 -based catalysts were prepared and loaded with Pd nanoparticles via an impregnation process. The Pd/H-TiO 2 catalyst demonstrated superior CO 2 reduction activity and a high formic acid production rate of 14.14 mmol cat ·g −1 ·h −1 . The excellent catalytic performance observed in the presence of a Pd/H-TiO 2 catalyst is ascribed to the synergy between O v and Pd. The presence of O v led to increase in CO 2 adsorption while Pd loading enhanced the photogenerated electron-hole pair separation. Electron transfer from H-TiO 2 to Pd also contributed to CO 2 activation.
研究领域:
环境科学
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材料科学
✓ 已验证
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
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2024
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IF 2.7
Wei Du,Min Li,Qiong Liu,Rong Chen
The electrocatalytic carbon dioxide reduction reaction (CO2RR) is considered as a promising approach for simultaneous CO2 treatment and production of value-added chemicals. Bismuth has been demonstrated as a fascinating electrocatalyst for selective conversion of CO2 to HCOOH. In this study, we comprehensively investigated the effects of size, morphology, and carbon supports on the CO2RR performance of Bi catalysts to enhance their electrocatalytic CO2RR activity and HCOOH selectivity. Specifically, Bi nanospheres with varying sizes were synthesized by adjusting the amount of polyvinylpyrrolidone (PVP), achieving similar selectivity for HCOOH but increasing current density with decreasing size. Bi nanoplates and Bi nanoflowers were also prepared through the reduction of BiOCl precursors, with Bi nanoflowers demonstrating a superior morphology compared to other Bi nanocrystals while achieving a HCOOH faradaic efficiency (FEHCOOH) of 95% at −1.6 V vs. SCE and excellent durability over 12 hours. The predominance of *HCOO intermediates in the in situ ATR-SEIRA spectra indicates that during the CO2RR, Bi nanoflowers primarily followed the pathway leading to HCOOH production. Furthermore, incorporation of Ketjenblack into the synthesis process resulted in carbon-supported Bi catalysts, which exhibited approximately 20% enhancement in FEHCOOH within a wide potential range from −1.3 V to −1.8 V vs. SCE due to an improved separation effect and electron transfer capacity provided by carbon materials.
研究领域:
电化学
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材料科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2023
·Vol. 33
·期 25
·2300547
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IF 19
Yin Zhu,Qizhu Qian,Yanxu Chen,Xiaoyue He,Xingwei Shi,Wentao Wang,Ziyun Li,Yafei Feng,Genqiang Zhang,Fangyi Cheng
Glycerol electrooxidation (GOR), as a typical nucleophile oxidation reaction, is deemed as a promising alternative anodic route to assist cathodic hydrogen evolution reaction. However, the investigations of high-performance catalysts and industrial-scale application of GOR remain a grand challenge. Herein, biphasic Ni 3 N/Co 3 N heterostructure nanowires (denoted as Ni 3 N/Co 3 N-NWs) are proposed as an efficient bifunctional catalyst, which realizes a high Faradaic efficiency of 94.6% toward formate production. Importantly, the flow electrolyzer achieves an industry-level current density of 1 A cm −2 at 2.01 V with impressive stability for steady running over 200 h, realizing lower electricity expense of 4.82 kWh m −3 H2 and energy saving efficiency of 9.7%, as well as outstanding co-production rates of 11 and 21.4 mmol cm −2 h −1 toward formate and H 2 , respectively. Theoretical calculations reveal that the efficient electron transfer on Ni 3 N/Co 3 N heterointerfaces simultaneously optimizes nucleophile reaction tendency and glycerol dehydrogenation kinetics, thus contributing to excellent GOR performance.
研究领域:
电化学
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催化材料
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能源转换
✓ 已验证
产品关联
DOI
高影响因子
GREEN CHEMISTRY
·
2024
·Vol. 26
·期 18
·9888-9898
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IF 9.3
Chongyan Chen,Shuguang Shen,Jie Wang,Yongmei Liu,Xingting Guo,Lili Zhang,Jing Li
The electroconversion of carbon dioxide (CO2) into value-added chemicals has attracted widespread attention worldwide. Exploring efficient catalysts and designing reasonable reactants have become popular research directions in the strategy of coupling anode and cathode reactions. Herein, we report the construction of a self-supporting bifunctional Sn–SnSx electrode using a one-step electrodeposition method. The valence states of Sn at the Sn–SnSx surface are Sn4+, Sn2+ and Sn0, and the electrode exhibits excellent performances for the carbon dioxide reduction reaction (CO2RR) and glucose oxidation reaction (GOR), respectively. For the CO2RR, the Sn–SnSx electrode produced formate with a faradaic efficiency (FE) of 93.3% and a stability of 36 h. Meanwhile, tin sulfides were first applied in anodic oxidation and a high FE of 88% was achieved for formate production in the GOR. Impressively, Sn–SnSx as a bifunctional electrode achieved co-production of formate at both the anode and cathode in the integrated electrolyzer coupled with the CO2RR and GOR. This coupling process combines the technical means of “electrooxidation–electroreduction” with the choice of reactants “CO2–C6H12O6”, resulting in FE values of 93.9% and 87.4% at the cathode and anode for the production of formate, as well as a 58.3% electrical energy saving for formate production in comparison with the traditional CO2RR coupled with the water oxidation reaction.
研究领域:
电化学
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催化材料
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能源转换
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
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2025
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IF 9.5
Ashfaq Ahamd,Chaoran Zhang,Yichuan Gu,Qu Jiang,Ziyang Sheng,Ruohan Feng,Sihong Wang,Haoyue Zhang,Qianqing Xu,Zijian Yuan,Fang Song
Ordered mesoporous materials offer significant advantages in reducing energy barriers, tuning intrinsic reaction pathways, and suppressing undesirable side reactions in electrocatalytic CO2 reduction reactions (CO2RR). Here, we present a straightforward method for the direct electrodeposition of ordered mesoporous CO2RR catalysts on a carbon-based porous transport layer, utilizing lyotropic liquid crystals (LLCs) as templates. The versatility of this method was demonstrated with tin-, bismuth-, and indium-based catalysts, all exhibiting pore sizes on the order of several nanometers. These ordered mesoporous catalysts efficiently and selectively drive CO2RR toward the value-added product of formate. They achieve partial current densities that are 3 to 8 times higher than those of disordered mesoporous reference samples, with a faradaic efficiency (FE) of up to 93% at an optimal potential of −0.9 V vs. RHE. In a flow cell configuration, Sn-based catalysts deliver a current density of ∼200 mA cm−2 over 22 hours at a potential of only −0.65 V vs. RHE. Spectroscopic and electrochemical analyses suggest that the high performance can be attributed to the exclusive exposure of active sites for the formate, improved mass transport, and modulated local microenvironments. Our work demonstrates a simple yet effective method for the direct deposition of efficient and selective catalysts onto electrodes. The insights gained from the underlying mechanisms provide valuable guidance for the design of high-performance CO2RR electrocatalysts.
研究领域:
材料科学
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电化学
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Zhaolin Shi,Chao Zhang,Hongjuan Wang,Zhouru Ji,Mengyu Qi,Simeng Liu,Weiqi Wang,Chen Chen,Jiqing Jiao,Tongbu Lu
Continuous production of liquid fuels in high concentration via electrocatalytic CO 2 reduction (CO 2 RR) calls for high-selectivity electrocatalysts and advanced devices. Here we designed and constructed a dual-functional heterojunction catalyst with an in situ growth strategy. The dual-functional heterojunction catalyst could synergistically activate CO 2 and water (as confirmed via in situ spectroscopy and theoretical calculations), and therefore the catalyst displayed a high selectivity and activity for formate production. Equipped with this catalyst, our custom-built gas–membrane–liquid electrolytic cell could continuously produce formate with a concentration as high as 1.55–1.85 M over the voltage range from 2.8 to 3.4 V (reaching the maximum of 1.85 M at 3.1 V). For continuous production of high-concentration HCOOH via CO 2 RR, our system features a broad voltage window. The results of theoretical calculations and in situ spectroscopies collectively demonstrate that constructing dual-functional heterojunction catalyst that work in synergy is the key solution to improving the overall catalytic performance.
研究领域:
电化学
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催化
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能量转换
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材料科学
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环境科学
✓ 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）