JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
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IF 8.128
Jialu Huang,Chengwei Deng,Yue Liu,Tingting Han,Feng Ji,Yuehua Zhang,Hongbin Lu,Ping Hua,Bowei Zhang,Tao Qian,Xiaolei Yuan,Yaoyue Yang,Yong Yao
Palladium (Pd) is supposed to be one of the most promising catalytic metals towards ethanol (C 2 H 5 OH) oxidation reaction (EOR). However, Pd electrocatalysts easily suffer from the poisoning of the intermediates (especially CO), resulting in the quick decay of EOR catalysis. Herein, inspired by the Brønsted-Lowry acid-base theory, a “attraction–repulsion” concept is proposed to guide the surface structure engineering toward EOR catalysts. Specifically, we induce Bi(OH) 3 species as Brønsted base onto PdBi nanoplates to effectively repel the adsorption of CO intermediates. The PdBi-Bi(OH) 3 nanoplates show an impressive mass activity of 4.46 A mg Pd -1 during the EOR catalysis and keep excellent stability. Both the stability and enhanced performance are attributed by the interfacial Brønsted base Bi(OH) 3 which can selectively attract and repel reactants and intermediates, as evidenced from in situ measurements and theoretical views.
研究领域:
材料科学
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电化学
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催化作用
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PubMed
高影响因子
ACS Nano
·
2025
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IF 16
Chengbo Li,Xian Zhong,Yuan Ji,Yawei Hong,Jiawei Li,Youpeng Wang,Hongliang Zeng,Chunxiao Liu,Zhaoyang Chen,Xu Li,Qiu Jiang,Tingting Zheng,Hong-Jie Peng,Xinyan Liu,Chuan Xia
The electrochemical conversion of CO2 into valuable chemicals under acidic conditions provides a promising solution to challenges, such as carbon loss and catalyst instability caused by carbonate precipitation. However, acidic CO2 electroreduction remains severely constrained by intense competition from the hydrogen evolution reaction (HER) and sluggish CO2 activation kinetics. Here, we report a bismuth (Bi) nanoparticle catalyst with an amorphous surface layer (a-Bi), which demonstrates high catalytic activity and selectivity toward formic acid (HCOOH) formation in acidic electrolytes. The catalyst achieves impressive Faradaic efficiencies for HCOOH production, exceeding 90% over a wide current density range (−100 to −1000 mA cm–2) with corresponding potentials ranging from −1.24 to −1.75 V versus the reversible hydrogen electrode (vs RHE). Notably, the partial current density for an HCOOH reaches an impressive value of more than −900 mA cm–2 at −1.75 V vs RHE. Furthermore, the a-Bi catalyst exhibited stability for over 52 h at high production rates (−500 mA cm–2) alongside a single-pass carbon efficiency of approximately 85%. In situ spectroscopy and theoretical simulation revealed that surface amorphization significantly enhances the adsorption of CO2 and lowers the hydrogenation barrier, thereby accelerating the CO2RR kinetics while effectively suppressing the HER. This work presents a facile crystallization engineering strategy to address critical carbon loss challenges, thereby advancing the sustainability and scalability of acidic CO2 electroreduction processes.
研究领域:
材料科学
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电化学
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能源转换
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DOI
PubMed
高影响因子
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
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2025
·Vol. 122
·期 10
·e2420922122
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IF 9.1
Zheng Chen,Yi Xiao,Xianji Qiao,Honghui Ou,Chi-Feng Lee,Hsiao-Tsu Wang,Yu-Cheng Shao,Lili Han
Although bismuth catalysts enable accelerated electrochemical CO2-to-formate conversion, the intrinsic active sites and forming mechanisms under operating conditions remain elusive. Herein, we prepared Bi2O2NCN, Bi2O3, and Bi2O2S as precatalysts. Among them, Bi2O2NCN-derived catalyst possesses optimum performance of electrochemical CO2-to-formate, exhibiting an upsurge of Faradaic efficiency to 98.3% at –0.6 V vs. reversible hydrogen electrodes. In-situ infrared and electrochemical impedance spectra trace and interpret the superior performance. Multimodal structural analyses utilizing quasi-in-situ X-ray diffraction, in-situ X-ray absorption near edge structure and in-situ Raman spectra provide powerful support to monitoring the catalysts’ in-situ transforms to metallic Bi, identifying the formation of the active sites influenced by the chalcogenide ions-guided: Carbodiimide promotes to form of the dominant Bi(003) facet exposure, which distinguishes from sulfide- and oxide-preferred dominant Bi(012) facets exposure. Concurrently, theoretical insights garnered from multiscale/multilevel computational analyses harmoniously corroborate the experimental findings. These findings show the pivotal role of chalcogenide in tailoring bismuth electrocatalysts for selective CO2 reduction to formate, illuminating the significance of controlling structural chemistry in designing catalysts toward high-efficiency renewable energy conversion.
研究领域:
电化学
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催化材料
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可再生能源
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DOI
PubMed
高影响因子
CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
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2025
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IF 3
Zhao Sirui,Zhou Heng,Cao Dengfeng,Sheng Beibei,Qian Fangren,Liu Chongjing,Chu Yongheng,Li Rongyao,Song Li,Chen Shuangming
Electrocatalytic reduction reaction of carbon dioxide (CO 2 RR) to formic acid is widely considered an effective strategy for addressing the greenhouse effect and enhancing energy conversion efficiency. However, existing catalytic systems are severely hampered by insufficient activity and significant hydrogen evolution reaction (HER), which substantially compromises the selectivity and stability of CO 2 RR, necessitating the development of highly efficient and stable electrocatalysts. Herein, we present a heteroatomic modification strategy to synthesize B-doped Bi and N-doped Bi electrocatalysts, and systematically investigate the regulation mechanism of incorporated elements on the electronic environment using X-ray absorption fine structure (XAFS) spectroscopy and other characterization techniques. The optimized B-doped Bi catalyst demonstrates exceptional catalytic performance, achieving a remarkable Faradaic efficiency of 95% for formic acid production at a high current density of −190 mA/cm 2 under alkaline conditions, while maintaining excellent stability for 20 h. Through comprehensive experimental characterization and theoretical calculations, we reveal that the B-doping-induced electron-rich structure significantly promotes CO 2 molecule activation and facilitates the formation of the key intermediate *OCHO, thereby achieving high selectivity and stability in CO 2 RR. This work not only elucidates the crucial role of electronic environment in CO 2 electrocatalytic conversion but also provides innovative insights into the rational design of high-performance electrocatalysts.
研究领域:
材料科学
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电化学
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DOI
高影响因子
NANO LETTERS
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2019
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IF 12.279
Xiaolei Yuan,Yong Zhang,Muhan Cao,Tong Zhou,Xiaojing Jiang,Jinxing Chen,Fenglei Lyu,Yong Xu,Jun Luo,Qiao Zhang,Yadong Yin
Developing high-performance electrocatalysts for the ethanol oxidation reaction (EOR) is critical to the commercialization of direct ethanol fuel cells. However, current EOR catalysts suffer from high cost, low activity, and poor durability. Here we report the preparation of PdBi-Bi(OH)3 composite nanochains with outstanding EOR activity and durability. The incorporation of Bi can tune the electronic structure and downshift the d-band center of Pd while the surface decoration of Bi(OH)3 can facilitate the oxidative removal of CO and other carbonaceous intermediates. As a result, the nanochains manifest an exceptional mass activity (5.30 A mgPd–1, 4.6-fold higher than that of commercial Pd/C) and outstanding durability (with a retained current density of ∼1.00 A mgPd–1 after operating for 20 000 s). More importantly, the nanochain catalyst can be reactivated, and negligible activity loss has been observed after operating for 200 000 s with periodic reactivation, making it one of the best EOR catalysts.
研究领域:
材料科学
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电化学
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DOI
PubMed
高影响因子
ChemCatChem
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2023
·Vol. 15
·期 19
·e202300703
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IF 4.5
Xinzheng Ma,Luyao Guo,Ziang Zhao,Yu Meng,Xiaoling Mou,Ronghe Lin,Yihui Li,Li Yan,Hejun Zhu,Yunjie Ding
Graphical Heptanol oxidation : Melamine modification of commercial activated carbon can greatly tune the performance of Pt−Bi catalysts in n -heptanol oxidation. C 3 N 4 -modified AC favors the formation of PtBi alloy in comparison to N-doped AC, and consequently boosts the activity and selectivity to heptanoic acid. Different bimetallic platinum and bismuth catalysts supported on melamine-modified activated carbon (AC) are designed by a co-impregnation method. Through controlling the activation temperatures of the melamine−AC mixture, a series of N-doped and C 3 N 4 -modified AC (N−AC and C 3 N 4 −AC) are prepared. Combined powder X-ray diffractions, X-ray photoelectron spectroscopic, and high-angle annual dark-field scanning transmission electron microscopic studies demonstrate that the introduction of C 3 N 4 favors the formation of PtBi alloy and leads to increased particle sizes in comparison to the pristine and N-doped AC-supported bimetallics. The catalytic performance of the developed catalysts is evaluated in the oxidation of n -heptanol oxidation in a batch mode using O 2 as the oxidant. PtBi/C 3 N 4 −AC exhibits significantly boosted activity as well as selectivity to heptanoic acid as compared with the other catalysts. A high yield of heptanoic acid of 69 % can be achieved under the optimized reaction conditions. Furthermore, our work points to the PtBi alloy as the most active sites for the alcohol oxidation. Catalyst deactivation occurs in the cycling tests, mainly due to the collapse of the alloy phase and likely the decrease in particle sizes.
研究领域:
催化化学
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材料科学
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
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IF 8.128
Wenshuang Lou,Luwei Peng,Ruinan He,Yuyu Liu,Jinli Qiao
Electrochemical reduction of CO 2 to fuels and chemicals is an effective way to reduce greenhouse gas emissions and alleviate the energy crisis, but the highly active catalysts necessary for this reaction under mild conditions are still rare. In this work, we grew CuBi bimetallic catalysts on derived copper foam substrates by co-electrodeposition, and then investigated the correlation between co-electrodeposition potential and electrochemical performance in CO 2 -to-formate conversion. Results showed that the bimetallic catalyst formed at a low potential of − 0.6 V vs. AgCl/Ag electrode achieved the highest formate Faradaic efficiency (FE formate ) of 94.4% and a current density of 38.5 mA/cm 2 at a low potential of − 0.97 V vs. reversible hydrogen electrode (RHE). Moreover, a continuous-flow membrane electrode assembly reactor also enabled the catalyst to show better performance (a FE formate of 98.3% at 56.6 mA/cm 2 ) than a traditional H-type reaction cell. This work highlights the vital impact of co-electrodeposition potential on catalyst performance and provides a basis for the modulated growth of bimetallic catalysts on substrates. It also shows the possibility of preparing Bi-based catalysts with no obvious decrease in catalytic activity that have been partially replaced with more economic copper.
研究领域:
化学
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能源科学
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环境科学
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DOI
PubMed
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-13
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IF 15.7
Chen Xingbao,Lu Ruihu,Li Chengbo,Luo Wen,Yu Ruohan,Zhu Jiexin,Lv Lei,Dai Yuhang,Gong Shanhe,Zhou Yazhou,Xiong Weiwei,Wu Jiahao,Cai Hongwei,Wu Xinfei,Deng Zhaohui,Xing Boyu,Su Lin,Wang Feiyue,Chao Feiyang,Chen Wei,Xia Chuan,Wang Ziyun,Mai Liqiang
Bi-defect sites are highly effective for CO 2 reduction (CO 2 RR) to formic acid, yet most catalytic surfaces predominantly feature inert, non-defective Bi sites. To overcome this limitation, herein, tensile strain is introduced on wholescale non-defective Bi sites. Under rapid thermal shock, the Bi-based metal-organic framework (Bi-MOF-TS) shows weakened Bi–O bonds and produced tiny Bi clusters. During electrochemical reduction, these clusters create numerous continuous vacancies, inducing weak tensile strain over a large range of surrounding non-defective Bi sites. This strain enhances *OHCO intermediates adsorption and substantially lowers the reaction barrier. As a result, Bi-MOF-TS achieves a faradaic efficiency above 90% across 800 mV potential range, with an impressive formate partial current density of −995 ± 93 mA cm −2 . Notably, Bi-MOF-TS exhibits a high HCOOH faradaic efficiency of 96 ± 0.64% at 400 mA cm −2 in acidic electrolyte and a high single-pass carbon conversion efficiency (SPCE) of 62.0%. Additionally, a Zn-CO 2 battery with Bi-MOF-TS as the cathode demonstrates a peak power density of 21.4 mW cm −2 and maintains stability over 300 cycles.
研究领域:
材料科学
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催化化学
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环境科学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Chenchen Weng,Cheng Wang,Yang Song,Yu-Xiao Zhang,Kang Zou,Hongwu Chen,Xue Yang,Wei Lin
The electrocatalytic CO 2 reduction reaction (CO 2 RR) to carbon-based fuels represents a promising strategy for carbon neutrality. Bi-based materials have emerged as leading candidates for CO 2 RR towards formate. However, dynamic reconstruction under actual CO 2 RR conduction imposes a challenge for the well-designed pristine Bi-based catalyst to deliver electrocatalytic activity. Herein, we report a high-efficient Bi catalyst which is in-situ formed via electrochemical activation of NO 3 − modulated Bi 2 O 2 CO 3 during CO 2 RR. The in-situ and ex-situ characterizations demonstrate that a directional reconstruction has been achieved under NO 3 − adjustment, in which the reinforced configuration focuses on the ordered Bi planar surface. The peak Faradaic efficiency for formate (FE HCOO − ) of 97 % is achieved at −0.9 V vs . RHE and a potential region with FE HCOO − over 90 % ranges from −0.7 to −1.1 V. Additionally, the formate partial current density reaches up to 329 mA cm −2 in a gas diffusion electrode configuration. The outstanding durability is evidenced through its stable and efficient formate production over 45 h. Moreover, the in-situ attenuated total reflection infrared and Raman analysis reveals that the *OCHO is the key intermediate for CO 2 RR towards formate and the in-situ generated Bi renders the favorable interaction with *OCHO intermediate, thus promoting CO 2 RR performance.
研究领域:
电化学
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材料科学
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催化反应
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产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
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2025
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IF 8.2
Shenao Wang,Yuan Yang,Yongtao Zhao,Jianwei Qiu,Xiaochen Wu,Zhaojun Liu,Fei Ding,Pengchao Si
Electrochemical reduction of CO2 (ECO2RR) to formate represents a promising approach to achieving carbon neutrality, yet it faces significant challenges due to the low adsorption efficiency of the CO2 intermediates. In this study, we developed a highly dispersed electron-rich Bi metal catalyst, utilizing low-cost g-C3N4 as a nonmetallic support and electron donor. This design created a conductive network and a multielectron environment around the Bi atoms that facilitated dynamic interfacial charge transfer from g-C3N4 to Bi, thus enhancing the catalytic efficiency of active sites. The assembly catalyst exhibited a formate selectivity of over 90% within a wide potential window and maintained stable catalytic activity in simulated seawater solutions. In situ Raman spectroscopy and DFT calculations indicated that the incorporation of the nonmetallic support shifted the Bi-p band center to more negative values while increasing Bader charge transfer between Bi and *OCHO intermediates. This indicated enhanced adsorption of the *OCHO intermediate by electron-rich Bi, thus improving the selectivity and activity for formate production.
研究领域:
材料科学
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环境科学
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催化化学
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产品关联
DOI
PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
·
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
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产品关联
DOI
高影响因子
Journal of Energy Chemistry
·
2025
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IF 14.9
Yipeng Nie,Zipei Cui,Longquan Deng,Zhuo Li,Shuo Chen,Wenchao Sheng
Electrocatalytic oxidation of glycerol for value-added chemicals is a superior strategy to utilize the excess glycerol produced in the biodiesel industry. Pd is one of the few active catalysts for alkaline glycerol oxidation reaction (GOR); however, glycerol inevitably dissociates and converts to carbon dioxide on the Pd surface, which results in its low total Faradaic efficiency (FE) for high-value-added products. Herein, a series of Pd/C and Pd 10 Bi x /C catalysts were synthesized to investigate the GOR pathway. The Pd 10 Bi 3 /C catalyst with optimal Bi content achieved an excellent GOR mass activity of 7.5±0.2 A mg Pd −1 and an outstanding total FE of 90%±3%, which are much higher than those values on Pd/C (1.2±0.2 A mg Pd −1 for mass activity and 63%±4% for total FE). Combined results of in-situ attenuated total reflection surface enhanced infrared absorption spectroscopy and density functional theory calculations show that Bi suppresses the dissociation of glycerol through the “shielding effect” of Bi to the adjacent Pd sites, which weakens the adsorption strength of GOR intermediates on those sites. This work provides a new insight into the GOR mechanism and puts forward a valid strategy for the rational design of catalysts to enable the transformation of glycerol into high-value-added products.
研究领域:
电催化
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能源化学
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材料化学
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表面科学
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可持续化学
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分子催化
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）